Devices comprising carbon-based material and fabrication thereof

ABSTRACT

Energy storage devices are disclosed. In some embodiments, the energy storage devices comprise a positive electrode comprising a carbon-based material comprising porous carbon sheet(s). Fabrication processes for manufacturing the energy storage devices are disclosed.

CROSS-REFERENCE

This application claims the benefit of U.S. Provisional Application No.62/381,859, filed Aug. 31, 2016, which application is incorporatedherein by reference.

BACKGROUND

As a result of the rapidly growing energy needs of modern life, thedevelopment of high-performance energy storage devices has gainedsignificant attention.

Lithium-ion batteries (LIBs) are very popular in portable electronicsbecause of their high energy density and small memory effect. They playan important role in the progress of electric vehicles, power tools, andmilitary and aerospace applications. LIBs in some cases dominate themarket for energy storage. However, like any other any storage system,LIBs still suffer from many shortcomings. While normal electronicdevices have seen very rapid progress following Moore's law, batterieshave advanced only slightly, mainly because of the lack of new materialswith high charge storage capacity.

SUMMARY

Recognized herein is the need for higher performance energy storagedevices (also “devices” herein). Provided herein are carbon-basedmaterials, fabrication processes, and devices with improved performance.

In some embodiments, the present disclosure provides batteries (e.g.,rechargeable batteries) that may avoid shortcomings of current batterytechnology. Provided herein are materials and fabrication processes ofsuch batteries. In some embodiments, carbon-based lithium-ion batteries(LIBs) that may avoid shortcomings of current LIB technology aredisclosed. Prototype carbon-based batteries disclosed herein may provideimproved performance compared with commercial LIB s. In certainembodiments, the batteries described herein may hold twice as muchcharge compared with commercial LIBs. The batteries described herein mayhave double the capacity of commercial cells, provide twice the power ofcommercial cells, have a cycle life and be used for twice as long, orany combination thereof. In certain embodiments, the batteries describedherein not only may have double the capacity of commercial cells butalso may provide twice the power and be used for twice as long.

The batteries described herein may play an important role in one or moreapplications or areas, for example, portable electronics (e.g.,cellphones, computers, and cameras), medical devices (e.g.,life-sustaining and life-enhancing medical devices, includingpacemakers, defibrillators, hearing aids, pain management devices, anddrug pumps), electric vehicles (e.g., batteries with long lifetime areneeded to improve the electric vehicles industry), space (e.g., thebatteries may be used in space to power space systems including rovers,landers, spacesuits, and electronic equipment), military batteries(e.g., the military uses special batteries for powering a large numberof electronics and equipment; the reduced mass and volume of thebatteries described herein are highly preferred), electric aircraft(e.g., an aircraft that runs on electric motors rather than internalcombustion engines, with electricity coming from solar cells orbatteries), grid scale energy storage (e.g., batteries may be used tostore electrical energy during times when production, from power plants,exceeds consumption and the stored energy may be used at times whenconsumption exceeds production), renewable energy (e.g., since the sundoes not shine at night and the wind does not blow at all times,batteries in off-the-grid power systems may store excess electricityfrom renewable energy sources for use during hours after sunset and whenthe wind is not blowing; high power batteries may harvest energy fromsolar cells with higher efficiency than current state-of-the-artbatteries), power tools (e.g., the batteries described herein may enablefast-charging cordless power tools such as drills, screwdrivers, saws,wrenches, and grinders; current batteries have a long recharging time),or any combination thereof.

Other goals and advantages of the device of the present disclosure willbe further appreciated and understood when considered in conjunctionwith the following description and accompanying drawings. While thefollowing description may contain specific details describing particularembodiments of the device of the present disclosure, this should not beconstrued as limitations to the scope of the device of the presentdisclosure but rather as an exemplification of preferable embodiments.For each aspect of the device of the present disclosure, many variationsare possible as suggested herein that are known to those of ordinaryskill in the art. A variety of changes and modifications may be madewithin the scope of the present disclosure without departing from thespirit thereof.

BRIEF DESCRIPTION OF DRAWINGS

The features of the device of the present disclosure are set forth withparticularity in the appended claims. A better understanding of thefeatures and advantages of the device of the present disclosure will beobtained by reference to the following detailed description that setsforth illustrative embodiments, in which the principles of the device ofthe present disclosure are utilized, and the accompanying drawings orfigures (also “FIG.” and “FIGs.” herein), of which:

FIG. 1 schematically illustrates an example of making porous carbonsheets.

FIG. 2 schematically illustrates an example of a fabrication process formanufacturing a battery comprising a carbon-based material in accordancewith the present disclosure.

FIG. 3 shows an example of coating of a slurry using large scaleroll-to-roll processing.

FIG. 4 shows an example of a process in which an aluminum foil is usedas a substrate and the process starts with unwinding the aluminum foilfor coating a slurry.

FIG. 5 shows an example of a close-up view of a slurry as it is beingcoated onto an aluminum foil/current collector (slurry is black).

FIG. 6 shows an example of an electrode/coated film after drying at 120°C. using an in-line heating oven.

FIG. 7 shows an example of rewinding an aluminum foil after it has beencoated.

FIG. 8 schematically illustrates examples of various carbon forms.

FIG. 9 is a schematic illustration of an example of a structure of abattery.

FIG. 10 shows an example of a fabrication process of a cell.

FIG. 11 shows examples of finished cells.

FIG. 12 shows an example of performance of an lithium iron phosphate(LFP)-based cell.

FIG. 13 is a schematic illustration of an example of a structure of abattery.

FIG. 14 shows an example of a fabrication process of a cell.

FIG. 15 shows examples of finished cells.

FIG. 16 shows an example of performance of a lithium nickel cobaltaluminum oxide (NCA)-based cell.

FIG. 17 is a schematic illustration of an example of a structure of abattery.

FIG. 18 is a bird's eye view of an example of an assembly process of acell.

FIG. 19 is a cross-sectional view of an example of an assembly processof a cell.

FIG. 20 shows an example of an assembly process of a cell.

FIG. 21 shows an example of a finished cell.

FIG. 22 shows an example of performance of a lithium nickel manganesecobalt oxide (NMC)-based cell.

FIG. 23 is a diagram showing an example of a Hummers'-based method(e.g., modified Hummers' method) of producing graphite oxide.

FIG. 24 is a diagram showing an example of a method for producinggraphite oxide.

FIG. 25 shows an exemplary method for coating a film with slurry.

FIG. 26 shows capacity measurements of exemplary energy storage devices.

FIG. 27 shows equivalent series resistance (ESR) measurements ofexemplary energy storage devices.

FIG. 28 shows exemplary dynamic ESR measurements of an exemplary energystorage device.

DETAILED DESCRIPTION

Provided herein are carbon-based materials, fabrication processes, anddevices with improved performance. In some embodiments, the presentdisclosure provides batteries (e.g., lithium-ion batteries (LIBs))comprising carbon-based material and their fabrication processes. Suchbatteries may avoid the shortcomings of current battery (e.g., LIB)technology. A battery of the present disclosure may comprise one or morebattery cells. A battery cell may comprise a positive electrode and anegative electrode separated by a separator comprising an electrolyte.The positive electrode may be a cathode during discharge. The negativeelectrode may be an anode during discharge.

In some embodiments, a plurality of battery cells may be arranged (e.g.,interconnected) in a battery pack. A large battery pack (e.g.,lithium-ion battery pack) may store the charge from rooftop solar panelsto provide power for home appliances. The large battery pack may helpstabilize the power grid. The large battery pack may lead to stand-alonepower systems that may work completely off the grid.

Carbon-Based Material

FIG. 8 schematically illustrates examples of various carbon forms 805,810, 815, 820, and 825. Such carbon forms may form various carbon-basedmaterials. The carbon forms may comprise functional groups. A givencarbon form may comprise, for example, one or more hydroxyl and/or epoxyfunctional groups 830, one or more carboxylic functional groups 835, oneor more other functional groups (e.g., carbonyl functional groups), orany combination thereof. The carbon form 805 may be, for example,graphite. The graphite may comprise a plurality of carbon sheets 840(e.g., greater than or equal to about 100, 1,000, 10,000, 100,000, 1million, 10 million, 100 million or more) that are each one atom thick.The plurality of carbon sheets 840 may be stacked on top of each other(e.g., as a result of strong van der Waals forces). The carbon sheets840 may stick together such that the interior of the stack may not beaccessible (e.g., only top and bottom sheets may be accessible, whilethe interior sheets stick together due to van der Waals interactionssuch that no pores are present). The carbon form 805 may includesubstantially no functional groups. The carbon form 810 may be, forexample, graphene. The graphene may comprise a carbon sheet 845 that isone atom thick. The carbon form 810 may include substantially nofunctional groups. The carbon form 815 may be, for example, grapheneoxide (e.g., singular graphite oxide in solution). The graphene oxidemay comprise a carbon sheet 850 that is one atom thick. In someembodiments, one or more carbon forms 815 may agglomerate. In suchinstances, individual carbon sheets 815 may be separated. The carbonsheets may not agglomerate due to van der Waals interactions. The carbonform 815 may include one or more hydroxyl and/or epoxy functional groups830, and one or more carboxylic functional groups 835. The hydroxyland/or epoxy functional groups 830 may be attached or otherwiseassociated with/bonded to the surfaces of the carbon sheet 850. Thecarboxylic functional groups 835 may be attached or otherwise associatedwith/bonded to edges of the carbon sheet 850. The carbon form 825 maybe, for example, few layer graphene oxide (e.g., bilayer or trilayergraphite oxide in solution). The few layer graphene oxide may comprisetwo or more carbon sheets or layers 860 that are each one atom thick.The two or more carbon sheets or layers 860 may be held together by vander Waals interactions. In some embodiments, the few layer grapheneoxide may comprise greater than or equal to 2, 3, 4, 5, 6, 7, 8, 9 or 10carbon sheets or layers 860. In an embodiment, the few layer grapheneoxide may comprise less than or equal to 10 carbon sheets or layers 860(e.g., up to 10 carbon sheets or layers). In some embodiments, the fewlayer graphene oxide may comprise between 2 and 3, 2 and 4, 2 and 5, 2and 6, 2 and 7, 2 and 8, 2 and 9, 2 and 10, 3 and 4, 3 and 5, 3 and 6, 3and 7, 3 and 8, 3 and 9, 3 and 10, 4 and 5, 4 and 6, 4 and 7, 4 and 8, 4and 9, 4 and 10, 5 and 6, 5 and 7, 5 and 8, 5 and 9, 5 and 10, 6 and 7,6 and 8, 6 and 9, 6 and 10, 7 and 8, 7 and 9, 7 and 10, 8 and 9, 8 and10, or 9 and 10 carbon sheets or layers 860. In some embodiments, thefew layer graphene oxide may comprise between 2 and 4, or 2 and 3 carbonsheets or layers 860. In an embodiment, the few layer graphene oxidecomprises up to 4 carbon sheets or layers 860. In another embodiment,the few layer graphene oxide comprises up to 4 carbon sheets or layers860. The carbon form 825 may include one or more carboxylic functionalgroups 835. The carboxylic functional groups 835 may be attached orotherwise associated with/bonded to edges of one or more of the carbonsheets 860. In some embodiments, the carboxylic functional groups 835may be primarily or solely attached or otherwise associated with/bondedto edges of the top and bottom carbon sheets 860 in a stack of thecarbon sheets or layers 860. In some embodiments, the carboxylicfunctional groups 835 may be attached or otherwise associatedwith/bonded to edges of any (e.g., each, or at least 2, 3, 4 or more) ofthe carbon sheets 860. The carbon form 820 may be, for example, reducedgraphene oxide (e.g., porous carbon sheets(s) (PCS) formed in solution).The reduced graphene oxide may comprise a carbon sheet 855 that is oneatom thick. The carbon form 820 may include one or more carboxylicfunctional groups 835. The carboxylic functional groups 835 may beattached or otherwise associated with/bonded to edges of the carbonsheet 855.

The presence and quantity of functional groups may affect the overallcarbon-to-oxygen (C:O) atomic ratio of the carbon forms in FIG. 8. Forexample, the carbon forms 825 and 815 may differ in the amount and/ortype of oxygen functionality. Such differences may affect theirrespective C:O atomic ratios. In another example, the carbon form 825may be produced upon oxidation of the carbon form 805, and the carbonform 825 may in turn be further oxidized to the carbon form 815. It willbe appreciated that each of the carbon forms in FIG. 8 may be producedvia one or more pathways, and/or at least some of the carbon forms inFIG. 8 may be transformed from one to another at least in someimplementations. For example, the carbon form 815 may be formed via analternative pathway.

In some embodiments, a single-layer graphite oxide and graphene oxide(GO) may comprise between about 93% and 96% (e.g., by weight) ofsingular graphene oxide (e.g., carbon form 815 in FIG. 8). In someembodiments, a multi-layer GO may comprise a given distribution (e.g.,by weight) of a number of layers (e.g., a distribution of carbon forms825 with different numbers of layers). For example, a multi-layer GO maycomprise greater than or equal to about 5%, 10%, 15%, 25%, 50%, 75%,85%, 90%, or 95% (e.g., by weight) of a carbon form 825 with a givennumber of layers (e.g., 3 or 4). The multi-layer GO may comprise suchpercentages of a carbon form 825 together with less than or equal toabout 95%, 90%, 75%, 50%, 25%, 15%, 10%, or 5% (e.g., by weight) ofanother carbon form 825 with a different number of layers. A multi-layerGO may comprise less than about 95%, 90%, 85%, 75%, 50%, 25%, 15%, 10%,or 5% (e.g., by weight) of a carbon form 825 with a given number oflayers.

In some instances, only edges of the graphite may be oxidized while thematerial maintains a large portion of the conductive properties ofgraphene (e.g., see carbon form 825 in FIG. 8). The GO from the firstreaction may have one or more properties (e.g., conductivity) that are,up to a given reaction time of the GO, substantially the same or similarto those of reduced GO. For example, the GO and reduced GO may besubstantially the same or similar in terms of one or more propertiesbelow a given degree of oxidation of the GO. In an example, whenoxidized (e.g., from the carbon form 805) to the carbon form 825, the GOmay have one or more properties that are substantially the same as orsimilar to reduced GO produced from one or more of the oxidized carbonforms in FIG. 8 (e.g., substantially the same as or similar to reducedGO produced from the carbon form 825). The GO may or may not maintainone or more of such properties upon further oxidation. For example, ifthe carbon form 825 is further oxidized to the carbon form 815, one ormore of such properties may differ (e.g., may begin to differ) from thereduced GO.

In some embodiments, the carbon-based material of the present disclosurecomprises one or more PCS. The carbon-based material may be dispersed insolution. For example, PCS may be formed through chemical reduction insolution (e.g., as described in greater detail elsewhere herein). A PCSmay have an oxygen content of less than or equal to about 10%, 9%, 8%,7%, 6%, 5%, 4.5%, 4%, 3.5%, 3%, 2.5%, 2%, 1.5%, 1%, or 0.5%. A PCS mayhave a pore size of less than or equal to about 10 nanometers (nm), 9nm, 8 nm, 7 nm, 6 nm, 5 nm, 4 nm, 3 nm, 2 nm, or 1 nm. A PCS may have apore size of greater than or equal to about 1 nm. A PCS may have a poresize of between about 1 nm and 2 nm, 1 nm and 3 nm, 1 nm and 4 nm, 1 nmand 5 nm, 1 nm and 6 nm, 1 nm and 7 nm, 1 nm and 8 nm, 1 nm and 9 nm, 1nm and 10 nm, 2 nm and 3 nm, 2 nm and 4 nm, 2 nm and 5 nm, 2 nm and 6nm, 2 nm and 7 nm, 2 nm and 8 nm, 2 nm and 9 nm, 2 nm and 10 nm, 3 nmand 4 nm, 3 nm and 5 nm, 3 nm and 6 nm, 3 nm and 7 nm, 3 nm and 8 nm, 3nm and 9 nm, 3 nm and 10 nm, 4 nm and 5 nm, 4 nm and 6 nm, 4 nm and 7nm, 4 nm and 8 nm, 4 nm and 9 nm, 4 nm and 10 nm, 5 nm and 6 nm, 5 nmand 7 nm, 5 nm and 8 nm, 5 nm and 9 nm, 5 nm and 10 nm, 6 nm and 7 nm, 6nm and 8 nm, 6 nm and 9 nm, 6 nm and 10 nm, 7 nm and 8 nm, 7 nm and 9nm, 7 nm and 10 nm, 8 nm and 9 nm, 8 nm and 10 nm, or 9 nm and 10 nm.For example, the PCS may have a pore size between about 1 nm and 4 nm,or 1 nm and 10 nm. The PCS may have one or more pore sizes (e.g., thePCS may have a distribution of such pore sizes).

Methods of Forming a Carbon-Based Material

FIG. 1 schematically illustrates an example of making PCS. Graphite 101may be chemically oxidized and exfoliated to graphite oxide or grapheneoxide 102. For the purpose of this disclosure, the terms graphite oxideand graphene oxide are used interchangeably. In some instances, graphiteoxide and graphene oxide are collectively referred to herein as “GO.”

The graphite 101 may be chemically oxidized and exfoliated to the GOusing Hummers' method and modified Hummers' method (and variousmodifications thereof, for example, various methods derived from themodified Hummers' method, including renamed methods derived from themodified Hummers' method), collectively referred to herein asHummers'-based methods.

In certain embodiments, a Hummers'-based method (e.g., a modifiedHummers' method) may require several weeks of purification, expensivehydrochloric acid (HCl) washes, proper technique that is left to thejudgment of the individual scientist, and/or a resulting product thatsometimes gives acceptable results and sometimes does not giveacceptable results.

FIG. 23 shows an example of a Hummers'-based method (e.g., a modifiedHummers' method) of producing graphite oxide. The method includes, in afirst step, adding 15 grams (g) graphite to 750 milliliters (mL)concentrated sulfuric acid (H₂SO₄) at 0° C. using an ice bath. Themethod further includes, in a second step, adding 90 g potassiumpermanganate (KMnO₄) (exothermic). A third step includes removing thereaction flask from the ice bath and waiting 2 hours. A fourth stepincludes placing the reaction flask back into the ice bath. In a fifthstep, 1.5 liters (L) water (H₂O) is added drop-wise over the course ofabout 1-1.5 hours while maintaining the temperature at 45° C.(controlling the temperature by the rate of addition of water and byadding ice to a melting ice bath). In certain embodiments, the ice bathfrom the first and/or second steps may be maintained and/or refilled foruse in the fourth and/or fifth steps. A sixth step includes removing thereaction flask from the ice bath and waiting 2 hours. A seventh stepincludes quenching the reaction with 4.2 L H₂O and then 75 mL 30%hydrogen peroxide (H₂O₂). An eighth step includes purification. Thepurification involves five HCl washes, followed by nine H₂O washes,followed by allowing the solution to air dry for about 2 weeks and thenrehydrating the dried graphite oxide with a known amount of water andputting it into dialysis for about 2 weeks. In an example, the totalprocessing time is about 2 months, and the total cost is $93/kg.

Alternatively, the graphite 101 may be chemically oxidized andexfoliated to the GO using a non-Hummers'-based method (e.g., firstreaction described in greater detail elsewhere herein). The GO may be ofdifferent forms (e.g., single-layer GO or multi-layer GO). The GO 102may be chemically reduced and activated to produce PCS 103. The PCS 103may comprise pores 104. The PCS may be a two-dimensional material.

In the non-Hummers'-based method, the graphite 101 may be chemicallyoxidized and exfoliated to the GO 102 in a first reaction. The firstreaction may be followed by a first purification. The GO 102 may bechemically reduced to the PCS 103 in a second reaction. The secondreaction may be followed by a second purification. In some embodiments,the first reaction and/or second reaction may allow GO and PCS,respectively, to be produced on a large scale (e.g., by the ton). Insome embodiments, the second reaction may be performed separately fromthe first reaction. For example, the second reaction, in some casesfollowed by the second filtration, may be performed using any graphiteoxide feedstock with suitable specifications.

The first reaction may include a low-temperature process for theproduction of GO with production of at least about 1 pound per day,including the time for purification. GO synthesis via the first reactionmay be tunable in terms of control of oxidation characteristics andamount of exfoliation, safer than other methods because of proceduraland engineered temperature controls, efficient in its minimal use ofreagents, configured to be fully scalable, or any combination thereof.In certain embodiments of the non-Hummers'-based method describedherein, the first reaction may produce a more controlled form of GO thanHummers'-based methods, as described in greater detail elsewhere herein.In some embodiments, this low-temperature process reduces the amount ofchemicals used and thus promises lower cost. In addition, the lowerreaction temperature of the method may reduce the risk of explosion.

The GO produced by the first reaction may be suitably exfoliated (e.g.,sufficiently exfoliated but not so much as to absorb a too large amountof water). The GO may have an amount and/or type of oxygen functionalitythat allows less than a given amount of water to be absorbed. The amountand type of oxygen functionality may change with degree of oxidation. Asdescribed elsewhere herein, GO produced using the first reactiondescribed herein may comprise a repeatable (e.g., consistent) amountand/or type of oxygen functionality. At least a portion of the oxygenfunctionality may allow water to be absorbed. The GO may besubstantially (e.g., fully) exfoliated but not over-oxidized. The GO maybe oxidized to a degree less than that which allows water to be absorbedin a suitably low amount (e.g., an over-oxidized graphite oxide maycomprise an excessive amount and/or unsuitable type(s) of oxygenfunctionality that allow an excessive amount of water to be absorbed).

In addition, the degree of oxidation of graphite oxide in the firstreaction may be adjusted to enable good control over the electricalconductivity and the number of layers of graphene oxide sheets in thefinal product. For example, reaction conditions may be adjusted to formsingle-layer graphite oxide or multi-layer graphite oxide. The two typesof graphite oxide may have different properties. The properties mayinclude, for example, given physicochemical properties and/orperformance characteristics (e.g., conductivity or purity). For example,single-layer graphite oxide or multi-layer graphite oxide may havedifferent conductive properties. In some embodiments, the resultinggraphite oxide synthesis product may be affected by reaction conditionsand/or by type or quality of the graphite feedstock.

A graphite feedstock may include various grades or purities, forexample, carbon content measured as, for example, weight-% graphiticcarbon (C_(g)), types (e.g., amorphous graphite, for example, 60%-85%carbon), flake graphite (e.g., greater than 85% carbon) or vein graphite(e.g., greater than 90% carbon), sizes (e.g., mesh size), shapes (e.g.,large flake, medium flake, powder, or spherical graphite), and origin(e.g., synthetic or natural, for example, natural flake graphite). Suchcharacteristics (e.g., physical and chemical properties) may affect thetype or quality of the graphite oxide. For example, the mesh size of thegraphite may affect the resulting graphite oxide. The graphite may havea grade or carbon content of at greater than or equal to about 1%, 2%,5%, 10%, 15%, 20%, 30%, 40%, 50%, 60%, 70%, 80%, 90%, 91%, 92%, 93%,94%, 95%, 96%, 97%, 98%, or 99% (e.g., by weight). The graphite may havea grade or carbon content of less than about 100%, 99%, 98%, 97%, 96%,95%, 94%, 93%, 92%, 91%, 90%, 85%, 80%, 70%, 60%, 50%, 40%, 30%, 20%,15%, 10%, 5%, 2%, or 1% (e.g., by weight). The graphite may have suchgrades or carbon contents at a mesh size of greater than or equal toabout −200, −150, −100, −80, −50, −48, +48, +80, +100, +150, or +200mesh size. Mesh sizes may be converted to size in other dimensions(e.g., microns). Other examples of graphite feedstocks are providedelsewhere herein.

The non-Hummers'-based GO synthesis method of the present disclosure maybe used to form GO with a given purity or grade (e.g., a minimum purityor grade). In some embodiments, purity or grade of the GO may beprovided in terms of an ionic conductivity measured at the end ofpurification. The ionic conductivity may provide a metric for how muchimpurity the graphite oxide contains. In some embodiments, the ionicconductivity (e.g., for the method in FIG. 24) may be between about 10microsiemens per centimeter (μS/cm) and 20 μS/cm, 10 μS/cm and 30 μS/cm,10 μS/cm and 40 μS/cm, 10 μS/cm and 50 μS/cm, 20 μS/cm and 30 μS/cm, 20μS/cm and 40 μS/cm, 20 μS/cm and 50 μS/cm, 30 μS/cm and 40 μS/cm, 30μS/cm and 50 μS/cm, or 40 μS/cm and 50 μS/cm. In some embodiments, theionic conductivity (e.g., for the method in FIG. 24) may be less thanand equal to about 50 μS/cm, 40 μS/cm, 30 μS/cm, 20 μS/cm or 10 μS/cm.In certain embodiments of the non-Hummers'-based method describedherein, the given purity or grade may be achieved at least about 2, 3,4, 5, 6, 7, 8, 9, or 10 times faster than a Hummers'-based method. Incertain embodiments of the non-Hummers'-based method described herein,the given purity or grade may be achieved between about 2 and 5, 2 and8, or 5 and 8 times faster than a Hummers'-based method. In certainembodiments of the non-Hummers'-based method described herein, thepurity or grade may be reached at the aforementioned faster ratesbecause a Hummers'-based method requires hydrochloric acid to be washedout and is therefore slower to reach the given purity or grade. Thesecond reaction may be used to form (e.g., from GO produced via thefirst reaction) PCS with a given purity or grade (e.g., a minimum purityor grade). In some embodiments, a purity or grade of the PCS may be atleast about 90%, 95%, 96%, 97%, 98%, 99%, 99.5%, or 99.9% carbon (e.g.,by weight).

In certain embodiments of the non-Hummers'-based method describedherein, the non-Hummers'-based method (e.g., see FIG. 24) may be faster,safer, and cheaper and may produce more repeatable results thanHummers'-based methods. In some embodiments, the improved repeatabilitymay be at least in part due to a lower reaction temperature than aHummers'-based method. In some embodiments, the non-Hummers'-basedmethod described herein produces GO with a composition (e.g., C:O atomicratio and quantity of oxygen functionality) and/or morphology repeatableto within about 1%, 2%, 3%, 4%, 5%, 6%, 7%, 8%, 9%, or 10%. For example,the method may produce GO with a C:O atomic ratio repeatable to withinabout 1%, 2%, 3%, 4%, 5%, 6%, 7%, 8%, 9%, or 10%. In certain embodimentsof the non-Hummers'-based method described herein, thenon-Hummers'-based method may include, for example, expeditedpurification without the use of costly HCl and a lower reactiontemperature that reduces the risk of explosion.

In certain embodiments of the non-Hummers'-based method describedherein, the non-Hummers'-based method may provide several advantages orbenefits over a Hummers'-based method. For example, in certainembodiments, the non-Hummers'-based method described herein may becheaper (e.g., at a cost per mass of graphite oxide of at least about 4times less than a Hummers'-based method; less waste per mass graphiteoxide produced than a Hummers'-based method), faster (e.g., removed HClwashes and/or faster purification; at least about 2, 5, or 8 timesfaster than (i) a Hummers'-based method or (ii) with HCl and/or withoutair drying; in less than or equal to about 1 week), more reliable (e.g.,removal of human error/judgment), safer (e.g., reaction runs at lowertemperatures, for example, at a maximum temperature of (i) less thanabout 45° C. or (ii) at least about 30° C. less than a maximumtemperature used in a Hummers'-based method), or any combinationthereof.

FIG. 24 is a diagram showing an example of a method for producinggraphite oxide. The method in FIG. 24 provides examples of the firstreaction and the first purification. The method includes, in a firststep, adding about 15 g graphite to about 750 mL concentrated H₂SO₄ atabout 0° C. using ice bath or recirculating chiller. In a second step,the method includes adding about 90 g KMnO₄ (exothermic) while keepingthe temperature below about 15° C. using an ice bath or recirculatingchiller. A third step (also “step 3” herein) includes stirring thereaction for about 45 minutes. A fourth step (also “step 4” herein)includes quenching the reaction by adding the reaction mixture to about2.6 kg ice and then adding about 75 mL 30% H₂O₂. The method may furtherinclude a fifth step comprising purification. In this example,purification involves five H₂O washes, followed by less than or equal toabout 1 week in a continuous-flow dialysis setup. In an example, thetotal processing time is about 1 week, and the total cost is $21/kg.

The reaction conditions (time/duration and temperature) in step 3 mayvary. In this example, the reaction in step 3 is cooled by ice bath, anda time of about 45 minutes is selected. In other examples, the durationmay be as described in greater detail elsewhere herein, and the reactiontemperature may vary with time (duration) according to specific coolingconditions (e.g., presence or absence of cooling by ice bath).

The purification in step 5 may include at least 1, 2, 3, 4, or 5 or moreH₂O washes. The purification in step 5 may include 5 or fewer H₂Owashes. The purification may further include other water purificationsteps, for example, dialysis. For example, dialysis may include placingthe material in a porous tube and removing (e.g., leaching out) ionsfrom the material through the walls of the tube into a water bath thatis refreshed continuously or batch-wise. The method may include usingone or more filtration methods other than dialysis (e.g., after the H₂Owashes, another filtration method may be applied in lieu of dialysis).The filtration may take less than 1 week. The duration of the filtrationmay depend on batch size. For example, for the 15 g graphite batchabove, filtration may take less than or equal to about 1 or 2 days.Total filtration (e.g., dialysis) time may be less than or equal toabout 7 days, 6 days, 5 days, 4 days, 3 days, 2 days, 1 day, or ½ day. Ashorter filtration time may reduce the total processing time to lessthan or equal to about 7 days, 6 days, 5 days, 4 days, 3 days, 2 days, 1day, or ½ day.

In step 4, the reaction mixture may be added to greater than or equal toabout 2.6 kg ice. In some instances, the amount of ice described hereinmay be a minimum amount. Step 4 may include adding greater than or equalto about 75 mL 30% H₂O₂. In some instances, the amount of H₂O₂ describedherein may be a minimum amount.

Given the scalability of the methods described herein (e.g., the methodin FIG. 24), the amount of oxidizing agent (also “oxidizer” herein) maybe provided in terms of a ratio of oxidizing agent (KMnO₄) to graphite(also “Ox:Gr” herein). For example, about 90 g KMnO₄ may be used per 15g graphite, corresponding to about 6× mass ratio Ox:Gr. In anotherexample, about 75 mL 30% H₂O₂ (e.g., about 30% by weight in aqueoussolution, corresponding to about 0.66 moles H₂O₂) may be used (i) per 90g KMnO₄, corresponding to about 0.25 units of H₂O₂ per unit of KMnO₄ ona weight basis or about 1.16 units of H₂O₂ per unit of KMnO₄ on a molarbasis, or (ii) per 750 mL concentrated H₂SO₄ with a concentration ofbetween about 96% H₂SO₄ and 98% H₂SO₄ (e.g., by weight in aqueoussolution), corresponding to a volume ratio of 30% H₂O₂ to concentratedsulfuric acid of about 10:1 (e.g., about 1 L of aqueous solution havingabout 30% H₂O₂ for every 10 L of concentrated H₂SO₄). In yet anotherexample, about 50 L of concentrated H₂SO₄ may be consumed for every 1 kgof graphite. Further examples of amounts and ratios are providedelsewhere herein, for example, in relation to methods for producingsingle-layer GO and multi-layer GO (e.g., on a per kilogram graphiteoxide basis).

In some embodiments, H₂SO₄ (e.g., with a concentration of between about96% H₂SO₄ and 98% H₂SO₄) may be provided in an amount between about 1 ggraphite:10 mL H₂SO₄ and about 1 g graphite:50 mL H₂SO₄. The method mayinclude providing between about 10 mL H₂SO₄ and 20 mL H₂SO₄, 10 mL H₂SO₄and 30 mL H₂SO₄, 10 mL H₂SO₄ and 40 mL H₂SO₄, 10 mL H₂SO₄ and 50 mLH₂SO₄, 20 mL H₂SO₄ and 30 mL H₂SO₄, 20 mL H₂SO₄ and 40 mL H₂SO₄, 20 mLH₂SO₄ and 50 mL H₂SO₄, 30 mL H₂SO₄ and 40 mL H₂SO₄, 30 mL H₂SO₄ and 50mL H₂SO₄, or 40 mL H₂SO₄ and 50 mL H₂SO₄ per 1 g graphite. The methodmay include providing greater than or equal to about 10 mL H₂SO₄, 20 mLH₂SO₄, 30 mL H₂SO₄, 40 mL H₂SO₄, or 50 mL H₂SO₄ per 1 g graphite. Themethod may include providing less than about 75 mL H₂SO₄, 70 mL H₂SO₄,60 mL H₂SO₄, 50 mL H₂SO₄, 40 mL H₂SO₄, 30 mL H₂SO₄, 20 mL H₂SO₄, or 15mL H₂SO₄ per 1 g graphite.

In some embodiments, H₂SO₄ (e.g., with a concentration of between about96% H₂SO₄ and 98% H₂SO₄) may be provided in an amount between about 1 ggraphite:18.4 g H₂SO₄ and about 1 g graphite:92.0 g H₂SO₄. The methodmay include providing between about 18.4 g H₂SO₄ and 30 g H₂SO₄, 18.4 gH₂SO₄ and 40 g H₂SO₄, 18.4 g H₂SO₄ and 50 g H₂SO₄, 18.4 g H₂SO₄ and 60 gH₂SO₄, 18.4 g H₂SO₄ and 70 g H₂SO₄, 18.4 g H₂SO₄ and 80 g H₂SO₄, 18.4 gH₂SO₄ and 92.0 g H₂SO₄, 30 g H₂SO₄ and 40 g H₂SO₄, 30 g H₂SO₄ and 50 gH₂SO₄, 30 g H₂SO₄ and 60 g H₂SO₄, 30 g H₂SO₄ and 70 g H₂SO₄, 30 g H₂SO₄and 80 g H₂SO₄, 30 g H₂SO₄ and 92.0 g H₂SO₄, 40 g H₂SO₄ and 50 g H₂SO₄,30 g H₂SO₄ and 60 g H₂SO₄, 30 g H₂SO₄ and 70 g H₂SO₄, 30 g H₂SO₄ and 80g H₂SO₄, 30 g H₂SO₄ and 92.0 g H₂SO₄, 40 g H₂SO₄ and 50 g H₂SO₄, 40 gH₂SO₄ and 60 g H₂SO₄, 40 g H₂SO₄ and 70 g H₂SO₄, 40 g H₂SO₄ and 80 gH₂SO₄, 40 g H₂SO₄ and 92.0 g H₂SO₄, 50 g H₂SO₄ and 60 g H₂SO₄, 50 gH₂SO₄ and 70 g H₂SO₄, 50 g H₂SO₄ and 80 g H₂SO₄, 50 g H₂SO₄ and 92.0 gH₂SO₄, 60 g H₂SO₄ and 70 g H₂SO₄, 60 g H₂SO₄ and 80 g H₂SO₄, 60 g H₂SO₄and 92.0 g H₂SO₄, 70 g H₂SO₄ and 80 g H₂SO₄, 70 g H₂SO₄ and 92.0 gH₂SO₄, 80 g H₂SO₄ and 92.0 g H₂SO₄ per 1 g graphite. The method mayinclude providing greater than or equal to about 18.4 g H₂SO₄, 20 gH₂SO₄, 25 g H₂SO₄, 30 g H₂SO₄, 35 g H₂SO₄, 40 g H₂SO₄, 45 g H₂SO₄, 50 gH₂SO₄, 55 g H₂SO₄, 60 g H₂SO₄, 65 g H₂SO₄, 70 g H₂SO₄, 75 g H₂SO₄, 80 gH₂SO₄, 85 g H₂SO₄, 90 g H₂SO₄, or 92.0 g H₂SO₄ per 1 g graphite. Themethod may include providing less than about 140 g H₂SO₄, 130 g H₂SO₄,120 g H₂SO₄, 110 g H₂SO₄, 100 g H₂SO₄, 95 g H₂SO₄, 90 g H₂SO₄, 80 gH₂SO₄, 70 g H₂SO₄, 60 g H₂SO₄, 50 g H₂SO₄, 40 g H₂SO₄, 30 g H₂SO₄, or 20g H₂SO₄ per 1 g graphite.

In some embodiments, KMnO₄ may be provided in an amount between about 1g graphite:2 g KMnO₄ and about 1 g graphite:6 g KMnO₄. The method mayinclude providing between about 1 g KMnO₄ and 2 g KMnO₄, 1 g KMnO₄ and 3g KMnO₄, 1 g KMnO₄ and 4 g KMnO₄, 1 g KMnO₄ and 5 g KMnO₄, 1 g KMnO₄ and6 g KMnO₄, 2 g KMnO₄ and 3 g KMnO₄, 2 g KMnO₄ and 4 g KMnO₄, 2 g KMnO₄and 5 g KMnO₄, 2 g KMnO₄ and 6 g KMnO₄, 3 g KMnO₄ and 4 g KMnO₄, 3 gKMnO₄ and 5 g KMnO₄, 3 g KMnO₄ and 6 g KMnO₄, 4 g KMnO₄ and 5 g KMnO₄, 4g KMnO₄ and 6 g KMnO₄, or 5 g KMnO₄ and 6 g KMnO₄ per 1 g graphite. Themethod may include providing greater than or equal to about 1 g KMnO₄, 2g KMnO₄, 3 g KMnO₄, 4 g KMnO₄, 5 g KMnO₄, or 6 g KMnO₄ per 1 g graphite.The method may include providing less than about 9 g KMnO₄, 8 g KMnO₄, 7g KMnO₄, 6 g KMnO₄, 5 g KMnO₄, 4 g KMnO₄, 3 g KMnO₄, or 2 g KMnO₄ per 1g graphite.

In some embodiments, H₂O₂ may be provided in an amount of at least about1 mol H₂O₂ per 1 mol KMnO₄. The method may include providing betweenabout 1 mol H₂O₂ and 1.1 mol H₂O₂, 1 mol H₂O₂ and 1.2 mol H₂O₂, 1 molH₂O₂ and 1.3 mol H₂O₂, 1 mol H₂O₂ and 1.4 mol H₂O₂, or 1 mol H₂O₂ and1.5 mol H₂O₂ per 1 mol KMnO₄. The method may include providing greaterthan or equal to about 1 mol H₂O₂, 1.1 mol H₂O₂, 1.2 mol H₂O₂, 1.3 molH₂O₂, 1.4 mol H₂O₂, or 1.5 mol H₂O₂ per 1 mol KMnO₄. The method mayinclude providing less than about 1.5 mol H₂O₂, 1.4 mol H₂O₂, 1.3 molH₂O₂, 1.2 mol H₂O₂, or 1.1 mol H₂O₂ per 1 mol KMnO₄.

In some embodiments, ice may be provided in an amount between about 1 gH₂SO₄:0 g ice and about 1 g H₂SO₄:1.09 g ice, between about 1 gH₂SO₄:1.09 g ice and about 1 g H₂SO₄:1.63 g ice, or between about 1 gH₂SO₄:0 g ice and about 1 g H₂SO₄:1.63 g ice. The method may includeproviding between about 0 g ice and 0.4 g ice, 0 g ice and 0.8 g ice, 0g ice and 1.2 g ice, 0 g ice and 1.63 g ice, 0.4 g ice and 0.8 g ice,0.4 g ice and 1.2 g ice, 0.4 g ice and 1.63 g ice, 0.8 g ice and 1.2 gice, 0.8 g ice and 1.63 g ice, or 1.2 g ice and 1.63 g ice per 1 gH₂SO₄. The method may include providing greater than or equal to about 0g ice, 0.2 g ice, 0.4 g ice, 0.6 g ice, 0.8 g ice, 1.09 g ice, 1.2 gice, 1.4 g ice, or 1.63 g ice per 1 g H₂SO₄. The method may includeproviding less than about 2.4 g ice, 2.2 g ice, 2.0 g ice, 1.8 g ice,1.63 g ice, 1.4 g ice, 1.2 g ice, 1.09 g ice, 0.8 g ice, 0.6 g ice, 0.4g ice, 0.2 g ice, or 0.1 g ice per 1 g H₂SO₄.

In some embodiments, ice may be provided in an amount between about 1 mLH₂SO₄:0 g ice and about 1 mL H₂SO₄:2 g ice, between about 1 mL H₂SO₄:2 gice and about 1 mL H₂SO₄:3 g ice, or between about 1 mL H₂SO₄:0 g iceand about 1 mL H₂SO₄:3 g ice. The method may include providing betweenabout 0 g ice and 1 g ice, 0 g ice and 2 g ice, 0 g ice and 3 g ice, 1 gice and 2 g ice, 1 g ice and 3 g ice, or 2 g ice and 3 g ice per 1 mLH₂SO₄. The method may include providing greater than or equal to about 0g ice, 0.2 g ice, 0.4 g ice, 0.6 g ice, 0.8 g ice, 1 g ice, 1.2 g ice,1.4 g ice, 1.6 g ice, 1.8 g ice, 2 g ice, 2.2 g ice, 2.4 g ice, 2.6 gice, 2.8 g ice or 3 g ice per 1 mL H₂SO₄. The method may includeproviding less than about 4.5 g ice, 4 g ice, 3.5 g ice, 3 g ice, 2.5 gice, 2 g ice, 1.5 g ice, 1 g ice, 0.5 g ice, 0.25 g ice, or 0.1 g iceper 1 mL H₂SO₄.

In certain embodiments, the graphite may be provided in powder form. Itwill be appreciated that the reactant amounts may be suitably scaled forproduction on a large scale. Substantially all of the graphite may beconverted. The amount of GO produced per unit of graphite may depend onthe oxygen content of the GO. In some embodiments, the C:O atomic ratioof the GO may be, for example, between about 4:1 and 5:1, and the amountof GO produced may be between about 1.27 and 1.33 units of GO per unitof graphite on a weight basis (e.g., between about 19 g and 20 g GO per15 g graphite). The C:O atomic ratio of the GO may differ forsingle-layer and multi-layer GO (e.g., as described in relation to FIG.8). Thus, the amount of GO produced per unit of graphite may differ forsingle-layer GO and multi-layer GOs. It will also be appreciated thatthe concentration of one or more of the reactants may in some casesvary. In an example, sulfuric acid may be provided at a concentration ofbetween about 96% H₂SO₄ and 98% H₂SO₄ (e.g., by weight in aqueoussolution). In another example, in some instances an absoluteconcentration of H₂O₂ may not substantially affect reaction conditions;instead, reaction conditions may depend on a ratio of H₂O₂ to KMnO₄(e.g., affecting lesser manganese species). In such instances, volumeand/or mass of the reactant mixture may be suitably adjusted such that agiven (e.g., predetermined) total mass or molar amount of the reactantis provided. It will further be appreciated that in some instances aminimum or maximum concentration may be required to ensure suitablereaction conditions. For example, a substantially lower sulfuric acidconcentration than about 96%-98% (e.g., by weight in aqueous solution)may lead to a different morphology of the GO (e.g., the lowerconcentration may affect oxygen-containing groups).

The present non-Hummers'-based method for producing graphite oxide maycomprise steps of: providing a graphite powder and H₂SO₄ mixture whilecooling the graphite powder and H₂SO₄ mixture to a first predeterminedtemperature; adding a predetermined amount of KMnO₄ to the graphitepowder and H₂SO₄ mixture to make a graphite oxidizing mixture; agitating(e.g., after the addition of the predetermined amount of KMnO₄ has beencompleted) the graphite oxidizing mixture for a predetermined amount oftime; cooling the graphite oxidizing mixture to a second predeterminedtemperature; and adding a predetermined amount of H₂O₂ to the graphiteoxidizing mixture to yield graphite oxide. In some implementations, thegraphite powder and H₂SO₄ mixture may be provided, and then cooled tothe first predetermined temperature.

The non-Hummers'-based method described herein may further includepurifying the graphite oxide by rinsing the graphite oxide with water(e.g., deionized water), purifying the graphite oxide by chemistrydialysis, or a combination thereof (e.g., rinsing followed by dialysis).

The first predetermined temperature resulting from cooling the graphitepowder and H₂SO₄ mixture may be about 0° C. The first predeterminedtemperature resulting from cooling the graphite powder and H₂SO₄ mixturemay range from about −10° C. to about 15° C. The first predeterminedtemperature may be greater than or equal to about −10° C., −9° C., −8°C., −7° C., −6° C., −5° C., −4° C., −3° C., −2° C., −1° C., or 0° C. butless than or equal to about 1° C., 2° C., 3° C., 4° C., 5° C., 6° C., 7°C., 8° C., 9° C., 10° C., 11° C., 12° C., 13° C., 14° C., or 15° C.

A reaction temperature of the graphite oxidizing mixture may beprevented from rising above about 15° C. while adding the predeterminedamount of KMnO₄ to the graphite powder and H₂SO₄ mixture. The additionof the KMnO₄ to the graphite powder and H₂SO₄ mixture may initiate anexothermic (e.g., self-heated) reaction. The reaction temperature of thegraphite oxidizing mixture may be less than or equal to about 15° C.,14° C., 13° C., 12° C., 11° C., 10° C., 9° C., 8° C., 7° C., 6° C., 5°C., 4° C., 3° C., 2° C., or 1° C. while adding the predetermined amountof KMnO₄ to the graphite powder and H₂SO₄ mixture. In certainembodiments, the reaction temperature of the graphite oxidizing mixturemay be less than about 15° C. while adding the predetermined amount ofKMnO₄ to the graphite powder and H₂SO₄ mixture.

The agitating may include stirring at a rate that ranges from about 50revolutions per minute (rpm) to about 150 rpm. In some embodiments, theagitating may include stirring at a rate of at least about 50 rpm, 60rpm, 70 rpm, 80 rpm, 90 rpm, 100 rpm, 110 rpm, 120 rpm, 130 rpm, 140rpm, or 150 rpm. In some embodiments, the agitating may include stirringat such rates (also “stirring rates” herein) while maintaining astirring rate of less than or equal to about 150 rpm. The predeterminedtime for agitating the graphite oxidizing mixture may range from about45 minutes to about 300 minutes. The predetermined time for agitatingthe graphite oxidizing mixture may be at least about 45 minutes, 50minutes, 60 minutes, 70 minutes, 80 minutes, 90 minutes, 100 minutes,120 minutes, 140 minutes, 160 minutes, 180 minutes, 200 minutes, 220minutes, 240 minutes, 260 minutes, 280 minutes, or 300 minutes. Thepredetermined time may or may not depend upon the stirring rate. In someexamples, the predetermined time may be independent of the stirring ratebeyond a given threshold (e.g., a minimum stirring rate) and/or within agiven range of stirring rates. In some embodiments, a reactiontemperature of the graphite oxidizing mixture during the agitating maybe maintained below about 45° C. In some embodiments, a reactiontemperature of the graphite oxidizing mixture during the agitating maybe maintained at less than or equal to about 15° C.

The cooling of the graphite oxidizing mixture to the secondpredetermined temperature may be achieved by quenching the graphiteoxidizing mixture with water and/or ice. The second predeterminedtemperature may be about 0° C. The second predetermined temperature mayrange from about 0° C. to about 10° C. The second predeterminedtemperature may be greater than or equal to about 0° C. but less than orequal to about 1° C., 2° C., 3° C., 4° C., 5° C., 6° C., 7° C., 8° C.,9° C., or 10° C.

In some embodiments, single-layer GO is produced. The first reaction mayinclude using about 32 L 98% H₂SO₄ per kilogram graphite. About 4.8 kgKMnO₄ powder per kilogram graphite may be used. The method may or maynot include cooking time. The method may include given temperatures andprocesses. The method may include, from the beginning of the reaction,about 1.5 hour of addition of KMnO₄ (reaction temperature less thanabout 15° C.), about 2 hours of reaction time (reaction temperaturerange of about 20-30° C.), about 1 hour of addition of about 32 kg ice(reaction temperature of about 50° C.) and about 1 hour reaction time(reaction temperature of about 50° C.). About 72 kg ice per kilogramgraphite may be used to quench the reaction and/or for ice for reactioncooling. About 2 L 30% H₂O₂ per kilogram of graphite may be used toquench the reaction and/or for neutralizing. The graphite may be of agiven type. The graphite may be 325sh natural flake graphite. Mixingspeed (e.g., during one or more reaction processes) may be about 100rpm. The method may include given timing of mixing ingredients. Sulfuricacid and graphite may be premixed to minimize graphite dust and added tothe reactor rapidly. Potassium permanganate addition may be exothermic.The KMnO₄ may be added at a rate slow enough to keep the reactiontemperature below about 15° C. (e.g., the KMnO₄ may be added overapproximately 1.5 hours).

During oxidation to single-layer GO, graphite (about 1 kg) may be mixedwith 98% H₂SO₄ (about 32 L) and chilled to about −10° C. GO reactorcooling coils may be chilled to −2° C. Graphite/H₂SO₄ mixture may thenbe poured carefully into the reactor. Potassium permanganate (about 4.8kg) powder may be added to the reactor slowly over the course of about1.5 hours, carefully keeping the reaction temperature below about 15° C.After addition of KMnO₄ is complete, the reactor cooling coiltemperature may be raised to about 12° C. and the reaction may heat upto about 30° C. over about 1.5 hours. Then, the reactor cooling coilsmay be cooled to about −2° C. and the reaction temperature may stay atabout 30° C. for approximately an additional 30 minutes. Crushed ice(about 32 kg) may be added over the course of about 1 hour. The reactiontemperature may climb to about 50° C. over this time. After iceaddition, the reaction may be allowed to stir for about 1 hour. Thereaction may then be quenched with crushed ice (about 72 kg). The icemay melt during this quench, and then 30% hydrogen peroxide (about 2 L)may be added to stop the reaction.

In some embodiments, multi-layer GO is produced. The first reaction mayinclude using about 25 L 98% H₂SO₄ per kilogram graphite. About 2 kgKMnO₄ per kilogram graphite oxide may be used. The method may or may notinclude cooking time. The method may include given temperatures andprocess(es). The method may include a 45-minute addition of KMnO₄(reaction temperature less than about 15° C.) and 30-minute reactiontime (reaction temperature of about 15° C.). About 125 kg ice perkilogram graphite may be used to quench the reaction and/or for ice forreaction cooling. About 1 L 30% hydrogen peroxide per kilogram ofgraphite may be used to quench the reaction and/or for neutralizing. Thegraphite may be of a given type. The graphite may be highly exfoliatedand milled, small flake, large surface area graphite, 9 micron flakes,or any combination thereof. Mixing speed (e.g., during one or morereaction processes) may be about 100 rpm. The method may include a giventiming of mixing ingredients. Sulfuric acid and graphite may be premixedto minimize graphite dust and added to the reactor rapidly. Potassiumpermanganate addition may be exothermic. The KMnO₄ may be added at arate slow enough to keep the reaction temperature below about 15° C.(e.g., the KMnO₄ may be added over approximately 1.5 hours).

During oxidation to multi-layer GO, graphite (about 1 kg) may be mixedwith 98% H₂SO₄ (about 32 L) and chilled to about −10° C. Graphiteoxide/graphene oxide reactor cooling coils may be chilled to about −2°C. Graphite/H₂SO₄ mixture may then be poured carefully into the reactor.Potassium permanganate (about 2 kg) powder may be added to the reactorslowly over the course of about 45 minutes, carefully keeping thereaction temperature below about 15° C. The reaction may then be allowedto stir for about 30 minutes at a reaction temperature of about 15° C.The reaction may then be quenched with crushed ice (about 125 kg). Theice may melt during this quench, and then 30% H₂O₂ (about 1 L) may beadded to stop the reaction.

A first purification may include filtration (also “first filtration”herein). The first filtration may be performed after the first reaction.The first filtration may include post-oxidation purification. The firstfiltration may remove impurities from the crude product and bring the pHup to at least about 5. After oxidation, the crude product may containGO as well as one or more (e.g., several) impurities, for example,H₂SO₄, manganese oxides, and manganese sulfate. After purification iscomplete, the GO may then be concentrated to, for example, a solution ofabout 1% by weight. Water and/or acid from first reaction may be removedduring filtration. After the first reaction, the acid concentration maybe about 30% (single-layer) or about 16% (multi-layer) H₂SO₄,corresponding to a pH of approximately 0. Filtration may be completewhen the pH reaches about 5, correspond to an acid concentration ofabout 0.00005%. A given amount or degree of concentration may be needed(e.g., if used as feedstock for a second reaction). In some embodiments,the GO may be in dry powder form and/or an aqueous solution of about 2%(by weight).

Purification may be performed using a tangential flow filtrationprocess. The filter type may be a modified polyether sulfone hollowfilter membrane with about 0.02 micron pore size. Purification may becomplete when the pH of the product reaches about 5. The purified GO maythen be concentrated to a solution of about 1% by weight. After thefirst purification, the H₂SO₄ concentration of the product may be about0.00005% with a pH of about 5.

The second reaction may include reduction of GO (in solution) to formreduced GO (e.g., PCS). In some embodiments, GO from the first reactionmay be used as input to the second reaction. For example, single-layerGO from the first reaction may be used as input to the second reaction.In some embodiments, GO produced by a Hummers'-based method may be usedas input to the second reaction. For example, single-layer GO from aHummers'-based method may be used as input to the second reaction. Insome embodiments, single-layer GO may be used instead of multi-layer GOas input to the second reaction to produce PCS. Use of single-layer mayin some instances reduce waste material relative to multi-layer GO whenPCS is produced in the second reaction (e.g., to produce sheets). Forexample, a higher amount of multi-layer GO may be needed to produce PCSthan when single-layer GO is used.

The second reaction may include heating the reaction to about 90° C. andadding H₂O₂ over the course of about an hour. The reaction may continueto heat at about 90° C. for about 3 more hours. Sodium ascorbate (e.g.,C₆H₇NaO₆) may be added over the course of about 30 minutes. The reactionmay continue to heat at about 90° C. for approximately an additional 1.5hours. The total time at about 90° C. may be about 6 hours. The mixingspeed (also “stirring rate” herein) may be as described elsewhere herein(e.g., in relation to synthesis of GO). In some embodiments, the mixingspeed (e.g., during one or more reaction processes) may be at leastabout 100 rpm, 110 rpm, 120 rpm, 130 rpm, 140 rpm, 150 rpm, 160 rpm, 170rpm, 180 rpm, 190 rpm, or 200 rpm.

As previously described, the reaction temperature may be about 90° C.Alternatively, one or more of the aforementioned steps may be performedat a temperature of between about 60° C. and 180° C. The steps may beperformed at the same temperature or temperature range, or at one ormore different temperatures or temperature ranges (e.g., at one or moredifferent temperatures between about 60° C. and 180° C.). For example,all steps may be performed at the same temperature (or temperaturerange), each step may be performed at a different temperature (ortemperature range), or subset(s) of steps may be performed at the sametemperature (or temperature range). In some embodiments, the temperaturemay be between about 60° C. and 80° C., 60° C. and 90° C., 60° C. and100° C., 60° C. and 120° C., 60° C. and 140° C., 60° C. and 160° C., 60°C. and 180° C., 80° C. and 90° C., 80° C. and 100° C., 80° C. and 120°C., 80° C. and 140° C., 80° C. and 160° C., 80° C. and 180° C., 90° C.and 100° C., 90° C. and 120° C., 90° C. and 140° C., 90° C. and 160° C.,90° C. and 180° C., 100° C. and 120° C., 100° C. and 140° C., 100° C.and 160° C., 100° C. and 180° C., 120° C. and 140° C., 120° C. and 160°C., 120° C. and 180° C., 140° C. and 160° C., 140° C. and 180° C., or160° C. and 180° C. The temperature may or may not be allowed to changeor fluctuate within a given range (e.g., the temperature for a givenstep may be kept constant at a given temperature within a given range,or may be allowed to fluctuate within the given range). In someinstances (e.g., at temperatures above about 100° C.), the reactionchamber may need to be sealed.

The concentration of the GO in the solution prior to the second reactionmay range, for example, between about 0% and 2% by mass (e.g., 0-2kg/100 L of aqueous solution). For example, the concentration of GO bymass may be between about 0% and 0.5%, 0% and 1%, 0% and 1.5%, 0% and2%, 0.5% and 1%, 0.5% and 1.5%, 0.5% and 2%, 1% and 1.5%, 1% and 2%, or1.5% and 2%. The concentration of GO may be less than or equal to about2%, 1.5%, 1%, 0.5%, 0.25%, 0.1% (or less) by mass. For example, theconcentration of GO in the solution (e.g., from the first reaction) maybe about 1% by mass (1 kg GO in 100 L of aqueous solution). In someembodiments, the concentration may be limited by how much GO may bedissolved in water while maintaining its fluidity. In some embodiments,the solution may become viscous (e.g., at a concentration of 2% or more,i.e., 2 kg or more of GO in 100 L of water). In some embodiments, thesolution viscosity may be less than a viscosity at which reactioncooking may become difficult. A higher concentration (e.g., 1% by mass)may allow the amount of water used in the reaction to be decreased(e.g., as high concentration as possible may minimize the amount ofwater used in the reaction). The water may be filtered at the end of thesecond reaction. A decrease in the amount of water used in the secondreaction may decrease filtration time (e.g., the larger the volume ofthe solution, the longer it may take in filtration).

In some embodiments, H₂O₂ (e.g., with a concentration of about 30% byweight) may be provided in an amount between about 10 L and 100 L per 1kg GO. For example, between about 10 L and 20 L, 10 L and 30 L, 10 L and40 L, 10 L and 50 L, 10 L and 60 L, 10 L and 70 L, 10 L and 80 L, 10 Land 90 L, 10 L and 100 L, 20 L and 30 L, 20 L and 40 L, 20 L and 50 L,20 L and 60 L, 20 L and 70 L, 20 L and 80 L, 20 L and 90 L, 20 L and 100L, 30 L and 40 L, 30 L and 50 L, 30 L and 60 L, 30 L and 70 L, 30 L and80 L, 30 L and 90 L, 30 L and 100 L, 40 L and 50 L, 40 L and 60 L, 40 Land 70 L, 40 L and 80 L, 40 L and 90 L, 40 L and 100 L, 50 L and 60 L,50 L and 70 L, 50 L and 80 L, 50 L and 90 L, 50 L and 100 L, 60 L and 70L, 60 L and 80 L, 60 L and 90 L, 60 L and 100 L, 70 L and 80 L, 70 L and90 L, 70 L and 100 L, 80 L and 90 L, 80 L and 100 L, or 90 L and 100 Lof H₂O₂ (e.g., with a concentration of about 30% by weight) may beprovided per 1 kg of GO. In some embodiments, greater than or equal toabout 10 L, 20 L, 30 L, 40 L, 50 L, 60 L, 70 L, 80 L, 90 L, or 100 L ofH₂O₂ (e.g., with a concentration of about 30% by weight) per 1 kg GO maybe provided. In some embodiments, less than about 100 L, 90 L, 80 L, 70L, 60 L, 50 L, 40 L, 30 L, 20 L, or 15 L of H₂O₂ (e.g., with aconcentration of about 30% by weight) per 1 kg GO may be provided. Anamount of H₂O₂ equivalent to any of the aforementioned amounts of the30% solution may be added as a solution with a different concentrationor in concentrated or pure form (e.g., 90%-100% by weight). The amountof H₂O₂ equivalent to any of the aforementioned amounts of the 30%solution may be expressed in terms of volume based on a 100% (or pure)solution. The amount of H₂O₂ equivalent to any of the aforementionedamounts of the 30% solution may be expressed in terms of moles or interms of weight of H₂O₂. For example, between about 3 kg (or 88 moles)and 30 kg (or 882 moles) of (pure) H₂O₂ may be provided per 1 kg GO.Expressed on a weight basis, between about 3 kg and 6 kg, 3 kg and 9 kg,3 kg and 12 kg, 3 kg and 15 kg, 3 kg and 18 kg, 3 kg and 21 kg, 3 kg and24 kg, 3 kg and 27 kg, 3 kg and 30 kg, 6 kg and 9 kg, 6 kg and 12 kg, 6kg and 15 kg, 6 kg and 18 kg, 6 kg and 21 kg, 6 kg and 24 kg, 6 kg and27 kg, 6 kg and 30 kg, 9 kg and 12 kg, 9 kg and 15 kg, 9 kg and 18 kg, 9kg and 21 kg, 9 kg and 24 kg, 9 kg and 30 kg, 12 kg and 15 kg, 12 kg and18 kg, 12 kg and 21 kg, 12 kg and 24 kg, 12 kg and 27 kg, 12 kg and 30kg, 15 kg and 18 kg, 15 kg and 21 kg, 15 kg and 24 kg, 15 kg and 30 kg,18 kg and 21 kg, 18 kg and 24 kg, 18 kg and 27 kg, 18 kg and 30 kg, 21kg and 24 kg, 21 kg and 27 kg, 21 kg and 30 kg, 24 kg and 27 kg, 24 kgand 30 kg, or 27 kg and 30 kg of pure H₂O₂ may be added per 1 kg GO.Expressed on a weight basis, greater than or equal to about 3 kg, 6 kg,9 kg, 12 kg, 15 kg, 18 kg, 21 kg, 24 kg, or 30 kg of pure H₂O₂ per 1 kgGO may be provided. Expressed on a weight basis, less than about 30 kg,24 kg, 21 kg, 18 kg, 15 kg, 12 kg, 9 kg, 6 kg, or 4.5 kg of pure H₂O₂per 1 kg GO may be provided.

In some embodiments, sodium ascorbate may be provided in an amountbetween about 1 kg and 10 kg per 1 kg GO. For example, between about 1kg and 2 kg, 1 kg and 3 kg, 1 kg and 4 kg, 1 kg and 5 kg, 1 kg and 6 kg,1 kg and 7 kg, 1 kg and 8 kg, 1 kg and 9 kg, 1 kg and 10 kg, 2 kg and 3kg, 2 kg and 4 kg, 2 kg and 5 kg, 2 kg and 6 kg, 2 kg and 7 kg, 2 kg and8 kg, 2 kg and 9 kg, 2 kg and 10 kg, 3 kg and 4 kg, 3 kg and 5 kg, 3 kgand 6 kg, 3 kg and 7 kg, 3 kg and 8 kg, 3 kg and 9 kg, 3 kg and 10 kg, 4kg and 5 kg, 4 kg and 6 kg, 4 kg and 7 kg, 4 kg and 8 kg, 4 kg and 9 kg,4 kg and 10 kg, 5 kg and 6 kg, 5 kg and 7 kg, 5 kg and 8 kg, 5 kg and 9kg, 5 kg and 10 kg, 6 kg and 7 kg, 6 kg and 8 kg, 6 kg and 9 kg, 6 kgand 10 kg, 7 kg and 8 kg, 7 kg and 9 kg, 7 kg and 10 kg, 8 kg and 9 kg,8 kg and 10 kg, or 9 kg and 10 kg of sodium ascorbate may be providedper 1 kg of GO. In some embodiments, greater than or equal to about 1kg, 2 kg, 3 kg, 4 kg, 5 kg, 6 kg, 7 kg, 8 kg, 9 kg or 10 kg of sodiumascorbate per 1 kg GO may be provided. In some embodiments, less thanabout 15 kg, 14 kg, 13 kg, 12 kg, 11 kg, 10 kg, 9 kg, 8 kg, 7 kg, 6 kg,5 kg, 4 kg, 3 kg, 2 kg or 1.5 kg of sodium ascorbate per 1 kg GO may beprovided.

In some embodiments, for 1 kg of GO, between about 10 L and 100 L of 30%H₂O₂ and between about 1 kg and 10 kg of sodium ascorbate may be used.

In some embodiments, at least about y=90%, 95%, 98%, 99%, or 99.5%, orsubstantially all of the GO may be converted. The amount of PCS producedper unit of GO may depend on the oxygen content of the GO and on theoxygen content of the PCS. In some embodiments, the C:O atomic ratio ofthe GO may be, for example, between about 4:1 and 5:1, and the oxygencontent of the PCS may be, for example, less than or equal to about 5atomic percent. In such cases, the amount of PCS produced may be betweenabout 0.75y and 0.84 units of PCS per unit of GO on a weight basis. Insome embodiments, the C:O atomic ratio of the GO may be, for example,between about 7:3 and 5:1, and the oxygen content of the PCS may be, forexample, less than or equal to about 5 atomic percent. In such cases,the amount of PCS produced may be between about 0.64y and 0.84 units ofPCS per unit of GO on a weight basis. In some embodiments, the C:Oatomic ratio of the GO may be, for example, at least about 7:3, and theoxygen content of the PCS may be, for example, less than or equal toabout 5 atomic percent. In such cases, the amount of PCS produced may beat least about 0.64y units of PCS per unit of GO on a weight basis. Insome embodiments, the amount of PCS produced may be at least about 0.5,0.55, 0.6, 0.65, 0.7, 0.75, or 0.8 units of PCS per unit of GO on aweight basis. In some embodiments, the amount of PCS produced may bebetween about 0.5 and 0.85, 0.6 and 0.8, or 0.7 and 0.8 units of PCS perunit of GO on a weight basis.

A second purification may include purifying PCS via vacuum filtrationthrough, for example, a 2 micron 316 stainless steel mesh filter. Thefiltration (also “second filtration” herein) may be performed after thesecond reaction. After the second reaction, there may be severalimpurities such as, for example, sodium ascorbate, plus small amounts ofH₂SO₄, manganese oxides, and manganese salts. The filtration may removeat least a portion of the impurities from the solution. Water, acid,and/or salts may be left over from second reaction. For example, theremay be about 4.95 kg of sodium ascorbate per kilogram of GO left over insolution from the second reaction. There may also be impurities from theGO. For example, there may remain small amounts of H₂SO₄, manganeseoxides, and manganese salts from the initial oxidation (e.g., firstreaction).

Water may be flushed through the PCS to remove salts. The conductivityof the solution after reduction may be greater than about 200millisiemens per centimeter (mS/cm). The PCS solution may be washed withdeionized water (e.g., with copious amounts of deionized water) untilthe conductivity of the PCS solution reaches about 50 microsiemens percentimeter (0/cm) or less. Purification may be complete when the PCSsolution has a conductivity of about 50 μS/cm or less. A given amount ordegree of concentration may be needed for straight PCS use. For example,a concentration of about 2% by weight or greater may be needed.

Energy Storage Devices

Energy storage devices of the present disclosure may comprise at leastone electrode (e.g., a positive electrode and a negative electrode). Thecarbon-based material of the present disclosure may be provided in thepositive electrode (cathode during discharge), the negative electrode(anode during discharge), or both. In certain embodiments, the energystorage device may be a lithium-ion battery. In certain embodiments, theenergy storage device may be a lithium metal battery. In certainembodiments, the energy storage device may be a supercapacitor.

A battery may comprise at least one cell comprising a negative electrode(anode during discharge) comprising graphite, and a positive electrode(cathode during discharge) comprising PCS/lithium iron phosphate (LFP).A configuration/form factor of the battery may be as described elsewhereherein (e.g., cylindrical, pouch, prismatic, or button cells of varioussizes). In certain embodiments, the battery may have a cylindricalconfiguration/form factor (e.g., 18650 packaging). It will beappreciated that while the positive electrode and battery in thisexample is primarily described as comprising PCS, such positiveelectrodes and batteries may comprise any carbon-based material inaccordance with the present disclosure.

FIG. 9 is a schematic illustration of an example of a structure of a(battery) cell (e.g., an LFP-based cell). The battery comprises apositive terminal 901, a gas release vent 902 adjacent to the positiveterminal 901, and a gasket 903 that seals the interior of the battery. Apositive tab 904 connects the positive terminal 901 to a positiveelectrode 907. A separator 906 separates the positive electrode from anegative electrode 905. In some embodiments, the battery compriseslayered sheets of, in sequence, the separator 906, the positiveelectrode 907, the separator 906, and the negative electrode 905 rolledinto a cylinder with a circular cross-section. In this configuration, atleast a portion of the outer surface of the cell (e.g., bottom surfaceof cell can) may serve as a negative terminal. FIG. 11 shows examples offinished LFP-based batteries. In this instance, the batteries areconfigured with a cylindrical configuration/form factor.

A battery may comprise at least one cell comprising a negative electrode(anode during discharge) comprising graphite, and a positive electrode(cathode during discharge) comprising PCS/lithium nickel cobalt aluminumoxide (NCA). A configuration/form factor of the battery may be asdescribed elsewhere herein (e.g., cylindrical, pouch, prismatic, orbutton cells of various sizes). In certain embodiments, the battery mayhave a cylindrical configuration/form factor (e.g., 18650 packaging).FIG. 16 shows example performance of an NCA-based battery. It will beappreciated that while the positive electrode and battery in thisexample is primarily described as comprising PCS, such positiveelectrodes and batteries may comprise any carbon-based material inaccordance with the present disclosure.

FIG. 13 is a schematic illustration of an example of a structure of a(battery) cell (e.g., an NCA-based cell). A side view 1301 and a topview 1302 of the battery are shown. In some embodiments, the battery hasa height of about 65 mm, and a diameter of about 18 mm. A separator 1312separates a cathode (positive electrode) 1313 from an anode (negativeelectrode) 1311. In some embodiments, the battery comprises layeredsheets of the anode 1311, the separator 1312, and the cathode 1313rolled into a cylinder with a circular cross-section. FIG. 15 showsexamples of finished NCA-based batteries. In this instance, thebatteries are configured with a cylindrical configuration/form factor.

A battery may comprise at least one cell comprising a negative electrode(anode during discharge) comprising graphite and a positive electrode(cathode during discharge) comprising PCS/lithium nickel manganesecobalt oxide (NMC). A configuration/form factor of the battery may be asdescribed elsewhere herein (e.g., cylindrical, pouch, prismatic, orbutton cells of various sizes). In certain embodiments, the battery mayhave a pouch configuration/form factor (e.g., LiPoly packaging). It willbe appreciated that while the positive electrode and battery in thisexample are primarily described as comprising PCS, such positiveelectrodes and batteries may comprise any carbon-based material inaccordance with the present disclosure.

FIG. 17 is a schematic illustration of an example of a structure of a(battery) cell (e.g., an NMC-based cell). A separator 1702 separates apositive electrode 1701 from a negative electrode 1703. In someembodiments, the battery comprises layered sheets of the negativeelectrode 1703, the separator 1702, and the positive electrode 1701rolled into a cylinder with a rectangular cross-section. The positiveand negative electrodes are connected with a positive tab 1704 and anegative tab 1705, respectively. The battery may be encapsulated in apreformed aluminum laminate 1706. FIG. 21 shows an example of a finishedNMC-based battery. In this instance, the battery is configured with apouch configuration/form factor.

Energy storage devices of the present disclosure may have differentconfigurations and/or form factors (e.g., see FIG. 9, FIG. 11, FIG. 13,FIG. 15, FIG. 17, and FIGS. 20-21). Any aspects of the presentdisclosure described in relation to a given configuration and/or formfactor described in relation to an energy storage device comprising agiven material or set of materials may equally apply to an energystorage device comprising a different material or set of materialsdescribed herein at least in some configurations. The energy storagedevices of the present disclosure may be packaged in any form. Thepackaging may be driven by final application.

A given configuration and/or form factor may include a given packaging.The configuration and/or form factor may be selected based onapplication (e.g., a pouch cell may be selected for application in acell phone, whereas cylindrical cells may be selected for certain otherconsumer devices). For example, a cell of an energy storage devicedescribed herein may be configured as a cylindrical cell, a pouch cell,a rectangular cell, a prismatic cell, a button cell, or anotherconfiguration. Each such configuration may have a given size and finalform factor. The form factor may correspond to a given packaging. Thepackaging may be rigid or non-rigid. The packaging may or may nothermetically seal the cell.

Cylindrical, prismatic, and button cells may use metallic enclosures. Acylindrical cell may have an exterior stainless steel can as itspackage. In some embodiments, a cell may comprise 18 mm by 65 mmcylindrical cell packaging (also “18650 packaging” herein), 26 mm by 65mm cylindrical cell packaging (also “26650 packaging” herein), or 32 mmby 65 mm cylindrical cell packaging (also “32650 packaging” herein).Such packaging may include, for example, one or more of outer metallicpackaging and a negative terminal (e.g., a cell can), gasket(s),insulator(s), separator(s) (e.g., anode separator(s)), a metal mesh,and/or other components (e.g., see FIG. 9 and FIG. 13). The sealed canexterior may withstand high internal pressures. In some embodiments, thecylindrical cell package may include a pressure relief mechanism, forexample, a membrane seal that ruptures upon excess internal pressure,and/or a re-sealable vent to release internal pressure.

A button cell may not have a safety vent. The button cell may comprise acell can (e.g., in electrical communication with a positive electrode)sealed to a cap (e.g., in electrical communication with a negativeelectrode) with a gasket.

Prismatic cells may be contained in a rectangular can. A prismatic cellmay be packaged, for example, in welded aluminum housings. Heavier gaugemetal may be used for a prismatic cell container (e.g., a slightlythicker wall size may be used for the prismatic cell to compensate fordecreased mechanical stability from a cylindrical configuration). Insome embodiments, electrodes of a prismatic cell may be stacked. In someembodiments, electrodes of a prismatic cell may be in the form of aflattened spiral. Prismatic cells may be configured in various formatsand/or sizes. Such formats and/or sizes may be configured, for example,based on charge storage capacity (e.g., 800 milliamp hours (mAh) to4,000 mAh format for mobile phones, tablets, low-profile laptops, andother portable consumer electronics, or 20-50 Ah for electricpowertrains in hybrid and electric vehicles).

Soft case/pack or pouch cells may comprise a laminated architecture in abag of thin aluminized plastic, glued with different types of polymersfor tightness. A pouch cell may comprise heat-sealable multi-layer foilpackaging (e.g., see FIG. 17). Such packaging may serve as a soft pack.The electrical contacts in the pouch cell may comprise conductive foiltabs welded to the electrodes and sealed to the pouch material (e.g.,brought to the outside in a fully sealed way). The pouch cell may bepackaged using, for example, lithium polymer battery packaging (e.g.,packaging used for lithium polymer cells with solid electrolytes, also“LiPoly packaging” herein). Such packaging may include, for example, afoil pouch with an outer plastic laminate. A pouch cell may havedifferent sizes. In some embodiments, a pouch cell may be configured orsized for a specific application (e.g., pouch cells may be placed intosmall areas between custom electronics packages). In some embodiments, asize of a pouch cell may correspond to given charge storage capacity(e.g., a charge storage capacity in the 40 Ah range for use in energystorage systems or a charge storage capacity suitable for cell phone andportable consumer electronics applications such as drones and hobbygadgets).

Composition of Energy Storage Devices

A lithium-ion battery (LIB) may comprise a negative electrode. In someembodiments, the LIB may comprise a carbon-based negative electrode(e.g., comprising graphite or carbon nanotubes). In some embodiments,the LIB may comprise a silicon (Si) negative electrode. In someembodiments, the LIB may comprise an alloy-based negative electrode(e.g., comprising tin alloys). In some embodiments, the LIB may comprisean oxide or sulfide-based negative electrode (e.g., comprisingmanganese(II) oxide (MnO) or magnesium sulfide (MgS)). The LIB maycomprise a positive electrode comprising an oxide, for example, layeredoxide (e.g., LiCoO₂), spinel (e.g., LiMn₂O₄), or olivine (e.g.,LiFePO₄). The LIB may comprise conductive additive(s). The conductiveadditive(s) may be provided in the positive electrode, the negativeelectrode, or both. The conductive additive(s) may include, for example,carbon black or carbon nanotubes. The LIB may comprise a binder, whereinthe binder comprises at least one of a first binder and a second binder.In some embodiments, the first binder is the same as the second binder.In some embodiments, the first binder is not the same as the secondbinder. The LIB may comprise an electrolyte. The electrolyte mayinclude, for example, a lithium salt (e.g., lithium hexafluorophosphate(LiPF₆), lithium tetrafluoroborate (LiBF₄), or lithium perchlorate(LiClO₄)) in an organic solution (e.g., ethylene carbonate, dimethylcarbonate, or diethyl carbonate).

In some embodiments, the carbon-based material of the present disclosuremay be provided in the positive electrode of a lithium-ion battery. Thecarbon-based material may be used as a conductive additive (e.g., toreplace carbon black). The carbon-based material may be used as anactive material in the positive electrode.

In some embodiments, the carbon-based material of the present disclosuremay be provided in the negative electrode of a lithium-ion battery. Thecarbon-based material may be used as an active material in the negativeelectrode. The carbon-based material may be used as coating on otheractive materials (e.g., Si) and/or may form composites with other activematerials (e.g., Si) for the negative electrode.

In some embodiments, the carbon-based material of the present disclosuremay be provided in the negative electrode of a lithium metal battery.The carbon-based material may be used as coating on the lithium negativeelectrode (e.g., to inhibit dendrite growth).

In some embodiments, the carbon-based material of the present disclosuremay be provided in the positive electrode and in the negative electrodeof a lithium-ion battery. The carbon-based material may be used as aconductive additive in the positive electrode and at the same time asactive material in the negative electrode. The carbon-based material maybe used as active material in the positive electrode (e.g., when GO isused in the negative electrode).

In some embodiments, the carbon-based material of the present disclosuremay be provided as active material in symmetric supercapacitors. Thecarbon-based material may be used in both electrodes (e.g., ascarbon-based aerogel).

In some embodiments, the carbon-based material of the present disclosuremay be provided as active material in asymmetric supercapacitors. Thecarbon-based material may be used as one electrode and coupled withanother electrode made of other materials (e.g., MnO₂). The carbon-basedmaterial may also be used in both electrodes when it forms compositeswith different materials in the two electrodes.

The energy storage devices described herein may comprise an electrolyte.Electrolytes described herein may include, for example, aqueous,organic, and/or ionic liquid-based electrolytes. The electrolyte may beliquid, solid, or a gel. An ionic liquid may be hybridized with anothersolid component, for example, polymer or silica (e.g., fumed silica), toform a gel-like electrolyte (also “ionogel” herein). An aqueouselectrolyte may be hybridized with, for example, a polymer, to form agel-like electrolyte (also “hydrogel” and “hydrogel-polymer” herein). Anorganic electrolyte may be hybridized with, for example, a polymer, toform a gel-like electrolyte. In some embodiments, the electrolyte mayalso include a lithium salt (e.g., LiPF₆, LiBF₄, or LiClO₄). Forexample, the electrolyte may include a lithium salt (e.g., LiPF₆, LiBF₄,or LiClO₄) in an organic solution (e.g., ethylene carbonate (EC),dimethyl carbonate (DMC), or diethyl carbonate (DEC)). The electrolytemay comprise one or more additional components (e.g., one or moreadditives). In some embodiments, an electrolyte composition (e.g., asoft pack polymer LIB electrolyte) may include one or more of EC, ethylmethyl carbonate (EMC), DEC, LiPF₆, and an additive. In someembodiments, an electrolyte composition (e.g., a high capacity LIBelectrolyte) may include one or more of EC, DEC, propylene carbonate(PC), LiPF₆, and an additive.

The energy storage device may comprise a polymer. In some embodiments,the energy storage device may comprise a separator. For example, theenergy storage device may comprise a polyethylene separator (e.g., anultra-high molecular weight polyethylene separator). The separator mayhave a thickness of less than or equal to about 16 μm, 15 μm, 14 μm, 13μm, 12 μm, 11 μm, 10 μm, 9 μm, or 8 μm (e.g., about 12±2.0 μm). Theseparator may have a given permeability. The separator may have apermeability (e.g., Gurley type) of greater than or equal to about 150sec/100 mL, 160 sec/100 mL, 170 sec/100 mL, 180 sec/100 mL, 190 sec/100mL, 200 sec/100 mL, 210 sec/100 mL, 220 sec/100 mL, 230 sec/100 mL, 240sec/100 mL, 250 sec/100 mL, 260 sec/100 mL, 270 sec/100 mL, 280 sec/100mL, 290 sec/100 mL, or 300 sec/100 mL (e.g., 180±50 sec/100 mL).Alternatively, the separator may have a permeability (e.g., Gurley type)of less than about 150 sec/100 mL, 160 sec/100 mL, 170 sec/100 mL, 180sec/100 mL, 190 sec/100 mL, 200 sec/100 mL, 210 sec/100 mL, 220 sec/100mL, 230 sec/100 mL, 240 sec/100 mL, 250 sec/100 mL, 260 sec/100 mL, 270sec/100 mL, 280 sec/100 mL, 290 sec/100 mL, or 300 sec/100 mL. Theseparator may have a given porosity. The separator may have a porosityof greater than or equal to about 35%, 40%, 45%, or 50% (e.g., 40%±5%).Alternatively, the separator may have a porosity of less than about 35%,40%, 45%, or 50%. The separator may have a given shut-down temperature(e.g., above the shut-down temperature, the separator may not functionnormally). In some embodiments, the separator may have a shut-downtemperature (actual) of less than or equal to about 150° C., 140° C.,130° C., 120° C., 110° C., or 100° C. In some embodiments, the separatormay have a shut-down temperature (DSC) between about 130° C. and 150°C., 130° C. and 140° C., or 136° C. and 140° C.

An active material of an electrode (e.g., a positive electrode of a LIB)may include, for example, graphene, lithium iron phosphate (LFP;LiFePO₄), lithium nickel cobalt aluminum oxide (NCA; LiNiCoAlO₂),lithium nickel manganese cobalt oxide (NMC; LiNiMnCoO₂), lithium cobaltoxide (LCO; LiCoO₂), lithium manganese oxide (LMO; LiMn₂O₄), lithiumtitanate (LTO; Li₄Ti₅O₁₂), lithium sulfur, or any combination thereof.One or more of such active materials may be present in the electrode atan individual or combined concentration (e.g., by weight on a dry basis,without solvent) between about 0.25% and 0.5%, 0.25% and 0.75%, 0.25%and 1%, 0.25% and 2%, 0.25% and 5%, 0.25% and 10%, 0.25% and 20%, 0.25%and 30%, 0.25% and 40%, 0.25% and 50%, 0.5% and 0.75%, 0.5% and 1%, 0.5%and 2%, 0.5% and 5%, 0.5% and 10%, 0.5% and 20%, 0.5% and 30%, 0.5% and40%, 0.5% and 50%, 0.75% and 1%, 0.75% and 2%, 0.75% and 5%, 0.75% and10%, 0.75% and 20%, 0.75% and 30%, 0.75% and 40%, 0.75% and 50%, 1% and2%, 1% and 5%, 1% and 10%, 1% and 20%, 1% and 30%, 1% and 40%, 1% and50%, 2% and 5%, 2% and 10%, 2% and 20%, 2% and 30%, 2% and 40%, 2% and50%, 5% and 10%, 5% and 20%, 5% and 30%, 5% and 40%, 5% and 50%, 10% and20%, 10% and 30%, 10% and 40%, 10% and 50%, 20% and 30%, 20% and 40%,20% and 50%, 30% and 40%, 30% and 50%, 40% and 50%, 50% and 55%, 50% and60%, 50% and 65%, 50% and 67%, 50% and 69%, 50% and 71%, 50% and 73%,50% and 75%, 50% and 77%, 50% and 79%, 50% and 81%, 50% and 83%, 50% and85%, 50% and 87%, 50% and 89%, 50% and 91%, 50% and 93%, 50% and 95%,50% and 97%, 50% and 99%, 55% and 60%, 55% and 65%, 55% and 67%, 55% and69%, 55% and 71%, 55% and 73%, 55% and 75%, 55% and 77%, 55% and 79%,55% and 81%, 55% and 83%, 55% and 85%, 55% and 87%, 55% and 89%, 55% and91%, 55% and 93%, 55% and 95%, 55% and 97%, 55% and 99%, 60% and 65%,60% and 67%, 60% and 69%, 60% and 71%, 60% and 73%, 60% and 75%, 60% and77%, 60% and 79%, 60% and 81%, 60% and 83%, 60% and 85%, 60% and 87%,60% and 89%, 60% and 91%, 60% and 93%, 60% and 95%, 60% and 97%, 60% and99%, 65% and 67%, 65% and 69%, 65% and 71%, 65% and 73%, 65% and 75%,65% and 77%, 65% and 79%, 65% and 81%, 65% and 83%, 65% and 85%, 65% and87%, 65% and 89%, 65% and 91%, 65% and 93%, 65% and 95%, 65% and 97%,65% and 99%, 67% and 69%, 67% and 71%, 67% and 73%, 67% and 75%, 67% and77%, 67% and 79%, 67% and 81%, 67% and 83%, 67% and 85%, 67% and 87%,67% and 89%, 67% and 91%, 67% and 93%, 67% and 95%, 67% and 97%, 67% and99%, 69% and 71%, 69% and 73%, 69% and 75%, 69% and 77%, 69% and 79%,69% and 81%, 69% and 83%, 69% and 85%, 69% and 87%, 69% and 89%, 69% and91%, 69% and 93%, 69% and 95%, 69% and 97%, 69% and 99%, 71% and 73%,71% and 75%, 71% and 77%, 71% and 79%, 71% and 81%, 71% and 83%, 71% and85%, 71% and 87%, 71% and 89%, 71% and 91%, 71% and 93%, 71% and 95%,71% and 97%, 71% and 99%, 73% and 75%, 73% and 77%, 73% and 79%, 73% and81%, 73% and 83%, 73% and 85%, 73% and 87%, 73% and 89%, 73% and 91%,73% and 93%, 73% and 95%, 73% and 97%, 73% and 99%, 75% and 77%, 75% and79%, 75% and 81%, 75% and 83%, 75% and 85%, 75% and 87%, 75% and 89%,75% and 91%, 75% and 93%, 75% and 95%, 75% and 97%, 75% and 99%, 77% and79%, 77% and 81%, 77% and 83%, 77% and 85%, 77% and 87%, 77% and 89%,77% and 91%, 77% and 93%, 77% and 95%, 77% and 97%, 77% and 99%, 79% and81%, 79% and 83%, 79% and 85%, 79% and 87%, 79% and 89%, 79% and 91%,79% and 93%, 79% and 95%, 79% and 97%, 79% and 99%, 81% and 83%, 81% and85%, 81% and 87%, 81% and 89%, 81% and 91%, 81% and 93%, 81% and 95%,81% and 97%, 81% and 99%, 83% and 85%, 83% and 87%, 83% and 89%, 83% and91%, 83% and 93%, 83% and 95%, 83% and 97%, 83% and 99%, 85% and 87%,85% and 89%, 85% and 91%, 85% and 93%, 85% and 95%, 85% and 97%, 85% and99%, 87% and 89%, 87% and 91%, 87% and 93%, 87% and 95%, 87% and 97%,87% and 99%, 89% and 91%, 89% and 93%, 89% and 95%, 89% and 97%, 89% and99%, 90% and 90.5%, 90% and 91%, 90% and 91.5%, 90% and 92%, 90% and92.5%, 90% and 93%, 90% and 93.5%, 90% and 94%, 90% and 94.5%, 90% and95%, 90% and 95.5%, 90% and 96%, 90% and 96.5%, 90% and 97%, 90% and97.5%, 90% and 98%, 90% and 98.5%, 90% and 99%, 90% and 99.5%, 90.5% and91%, 90.5% and 91.5%, 90.5% and 92%, 90.5% and 92.5%, 90.5% and 93%,90.5% and 93.5%, 90.5% and 94%, 90.5% and 94.5%, 90.5% and 95%, 90.5%and 95.5%, 90.5% and 96%, 90.5% and 96.5%, 90.5% and 97%, 90.5% and97.5%, 90.5% and 98%, 90.5% and 98.5%, 90.5% and 99%, 90.5% and 99.5%,91% and 91.5%, 91% and 92%, 91% and 92.5%, 91% and 93%, 91% and 93.5%,91% and 94%, 91% and 94.5%, 91% and 95%, 91% and 95.5%, 91% and 96%, 91%and 96.5%, 91% and 97%, 91% and 97.5%, 91% and 98%, 91% and 98.5%, 91%and 99%, 91% and 99.5%, 91.5% and 92%, 91.5% and 92.5%, 91.5% and 93%,91.5% and 93.5%, 91.5% and 94%, 91.5% and 94.5%, 91.5% and 95%, 91.5%and 95.5%, 91.5% and 96%, 91.5% and 96.5%, 91.5% and 97%, 91.5% and97.5%, 91.5% and 98%, 91.5% and 98.5%, 91.5% and 99%, 91.5% and 99.5%,92% and 92.5%, 92% and 93%, 92% and 93.5%, 92% and 94%, 92% and 94.5%,92% and 95%, 92% and 95.5%, 92% and 96%, 92% and 96.5%, 92% and 97%, 92%and 97.5%, 92% and 98%, 92% and 98.5%, 92% and 99%, 92% and 99.5%, 92.5%and 93%, 92.5% and 93.5%, 92.5% and 94%, 92.5% and 94.5%, 92.5% and 95%,92.5% and 95.5%, 92.5% and 96%, 92.5% and 96.5%, 92.5% and 97%, 92.5%and 97.5%, 92.5% and 98%, 92.5% and 98.5%, 92.5% and 99%, 92.5% and99.5%, 93% and 93.5%, 93% and 94%, 93% and 94.5%, 93% and 95%, 93% and95.5%, 93% and 96%, 93% and 96.5%, 93% and 97%, 93% and 97.5%, 93% and98%, 93% and 98.5%, 93% and 99%, 93% and 99.5%, 93.5% and 94%, 93.5% and94.5%, 93.5% and 95%, 93.5% and 95.5%, 93.5% and 96%, 93.5% and 96.5%,93.5% and 97%, 93.5% and 97.5%, 93.5% and 98%, 93.5% and 98.5%, 93.5%and 99%, 93.5% and 99.5%, 94% and 94.5%, 94% and 95%, 94% and 95.5%, 94%and 96%, 94% and 96.5%, 94% and 97%, 94% and 97.5%, 94% and 98%, 94% and98.5%, 94% and 99%, 94% and 99.5%, 94.5% and 95%, 94.5% and 95.5%, 94.5%and 96%, 94.5% and 96.5%, 94.5% and 97%, 94.5% and 97.5%, 94.5% and 98%,94.5% and 98.5%, 94.5% and 99%, 94.5% and 99.5%, 95% and 95.5%, 95% and96%, 95% and 96.5%, 95% and 97%, 95% and 97.5%, 95% and 98%, 95% and98.5%, 95% and 99%, 95% and 99.5%, 95.5% and 96%, 95.5% and 96.5%, 95.5%and 97%, 95.5% and 97.5%, 95.5% and 98%, 95.5% and 98.5%, 95.5% and 99%,95.5% and 99.5%, 96% and 96.5%, 96% and 97%, 96% and 97.5%, 96% and 98%,96% and 98.5%, 96% and 99%, 96% and 99.5%, 96.5% and 97%, 96.5% and97.5%, 96.5% and 98%, 96.5% and 98.5%, 96.5% and 99%, 96.5% and 99.5%,97% and 97.5%, 97% and 98%, 97% and 98.5%, 97% and 99%, 97% and 99.5%,97.5% and 98%, 97.5% and 98.5%, 97.5% and 99%, 97.5% and 99.5%, 98% and98.5%, 98% and 99%, 98% and 99.5%, 98.5% and 99%, 98.5% and 99.5%, or99% and 99.5%. One or more of such active materials may be present inthe electrode at an individual or combined concentration (e.g., byweight on a dry basis, without solvent) of greater than or equal toabout 50%, 51%, 52%, 53%, 54%, 55%, 56%, 57%, 58%, 59%, 60%, 61%, 62%,63%, 64%, 65%, 65.5%, 66%, 66.5%, 67%, 67.5%, 68%, 68.5%, 69%, 69.5%,70%, 70.5%, 71%, 71.5%, 72%, 72.5%, 73%, 73.5%, 74%, 74.5%, 75%, 75.5%,76%, 76.5%, 77%, 77.5%, 78%, 78.5%, 79%, 79.5%, 80%, 80.5%, 81%, 81.5%,82%, 82.5%, 83%, 83.5%, 84%, 84.5%, 85%, 85.5%, 86%, 86.5%, 87%, 87.5%,88%, 88.5%, 89%, 89.5%, 90%, 90.5%, 91%, 91.5%, 92%, 92.5%, 93%, 93.5%,94%, 94.5%, 95%, 95.5%, 96%, 96.5%, 97%, 97.5%, 98%, 98.5%, 99%, 99.5%,or 99.9%. In addition, or as an alternative, one or more of such activematerials may be present in the electrode at an individual or combinedconcentration of less than or equal to about 99.9%, 99.5%, 99%, 98.5%,98%, 97.5%, 97%, 96.5%, 96%, 95.5%, 95%, 94.5%, 94%, 93.5%, 93%, 92.5%,92%, 91.5%, 91%, 90.5%, 90%, 89.5%, 89%, 88.5%, 88%, 87.5%, 87%, 86.5%,86%, 85.5%, 85%, 84.5%, 84%, 83.5%, 83%, 82.5%, 82%, 81.5%, 81%, 80.5%,80%, 79.5%, 79%, 78.5%, 78%, 77.5%, 77%, 76.5%, 76%, 75.5%, 75%, 74.5%,74%, 73.5%, 73%, 72.5%, 72%, 71.5%, 71%, 70.5%, 70%, 69.5%, 69%, 68.5%,68%, 67.5%, 67%, 66.5%, 66%, 65.5%, 65%, 64%, 63%, 62%, 61%, 60%, 59%,58%, 57%, 56%, 55%, 54%, 53%, 52%, 51%, or 50%. One or more of suchactive materials may be present in the electrode at such concentrationsin combination with one or more other materials (e.g., one or more otherelectrode materials and concentrations thereof described herein).

The aforementioned active material may comprise non-lithium metals at agiven ratio. For example, the active material may comprise nickel,cobalt, and aluminum at a given ratio (e.g., about 0.815:0.15:0.035 forNCA), or nickel, cobalt, and manganese at a given ratio (e.g., about6:2:2 for NMC). The active material may comprise at least 1, 2, 3, 4, 5,or more non-lithium metals. The non-lithium metals may be selectedamong, for example, nickel, cobalt, aluminum, manganese, iron, andtitanium. In some embodiments, the active material may comprise a firstnon-lithium metal at a ratio (e.g., by weight or by mol) of at leastabout 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, or 15 with respect to a secondnon-lithium metal. In some embodiments, the active material may comprisethe first non-lithium metal at a ratio (e.g., by weight or by mol) of atleast about 1, 2, 3, 4, 5, 6, 8, 10, 12, 14, 16, 18, 20, 22, 24, 26, 28,30, or 35 with respect a third non-lithium metal. In some embodiments,the active material may comprise the second non-lithium metal at a ratio(e.g., by weight or by mol) of at least about 1, 2, 3, 4, 5, 6, 7, 8, 9,10, or 15 with respect to the third non-lithium metal. The activematerial may comprise the non-lithium metal(s) and/or one or morenon-metals at an individual or combined concentration (e.g., by weight)of greater than or equal to about 1%, 2%, 4%, 6%, 8%, 10%, 15%, 20%,25%, 30%, 35%, 40%, 45%, 50%, 55%, 60%, 65%, 70%, 75%, 80%, 85%, 90%,95%, or 99%. In addition, or as an alternative, the active material maycomprise the non-lithium metal(s) and/or the one or more non-metals atan individual or combined concentration (e.g., by weight) of less thanor equal to about 99.5%, 99%, 95%, 90%, 85%, 80%, 75%, 70%, 65%, 60%,55%, 50%, 45%, 40%, 35%, 30%, 25%, 20%, 15%, 10%, 5%, or 2%. In certainembodiments, the active material may comprise nickel, cobalt, andaluminum at a concentration (e.g., by weight total) of at least about50%, 51%, 52%, 53%, 54%, 55%, 56%, 57%, 58%, 59%, or 60% (e.g., about59±1.0% for NCA). In certain embodiments, the active material maycomprise iron at a concentration (e.g., by weight) between about 33% and36%, and phosphorus at a concentration (e.g., by weight) between about19% and 21% (e.g., greater than or equal to about 58.5% for NMC). Incertain embodiments, the active material may comprise nickel, cobalt,and aluminum at a concentration (e.g., by weight total) of at leastabout 50%, 51%, 52%, 53%, 54%, 55%, 56%, 57%, 58%, 59%, or 60% (e.g.,about 59±1.0% for NCA). The active material may comprise lithium at aconcentration (e.g., by weight) of at greater than or equal to about 1%,1.5%, 2%, 2.5%, 3%, 3.5%, 4%, 4.5%, 5%, 5.5%, 6%, 6.5%, 7%, 7.5%, 8%,8.5%, 9%, 9.5%, or 10%. In addition, or as an alternative, the activematerial may comprise lithium at a concentration (e.g., by weight) ofless than or equal to about 15%, 10%, 8%, 6%, 5%, 4%, 3%, 2%, or 1.5%.For example, the active material may comprise lithium at a concentration(e.g., by weight) of about 7.2±0.4% for NCA, 7.1% for NMC, or betweenabout 3.9% and 4.9% for LFP. The active material may comprise suchlithium concentrations in addition to the aforementioned concentrationsof non-lithium metals (e.g., of nickel, cobalt, and aluminum, or ofnickel, cobalt, and manganese). The active material may have a givenspecific surface area. The active material may have a specific surfacearea greater than or equal to about 0.1 square meter per gram (m²/g),0.2 m²/g, 0.3 m²/g, 0.4 m²/g, 0.5 m²/g, 0.6 m²/g, 0.7 m²/g, 0.8 m²/g,0.9 m²/g, 1 m²/g, 2 m²/g, 3 m²/g, 4 m²/g, 5 m²/g, 6 m²/g, 7 m²/g, 8m²/g, 9 m²/g, 10 m²/g, 11 m²/g, 12 m²/g, 13 m²/g, 14 m²/g, 15 m²/g, 16m²/g, 17 m²/g, 18 m²/g, 19 m²/g, 20 m²/g or 25 m²/g. In addition, or asan alternative, the active material may have a specific surface area ofless than or equal to about 30 m²/g, 25 m²/g, 20 m²/g, 19 m²/g, 18 m²/g,17 m²/g, 16 m²/g, 15 m²/g, 14 m²/g, 13 m²/g, 12 m²/g, 11 m²/g, 10 m²/g,9 m²/g, 8 m²/g, 7 m²/g, 6 m²/g, 5 m²/g, 4 m²/g, 3 m²/g, 2 m²/g, 1 m²/g,0.9 m²/g, 0.8 m²/g, 0.7 m²/g, 0.6 m²/g, 0.5 m²/g, 0.4 m²/g, 0.3 m²/g, or0.2 m²/g. In some embodiments, the active material (e.g., NCA) may havea specific surface area between about 0.3 m²/g and 0.7 m²/g. In someembodiments, the active material (e.g., NMC) may have a specific surfacearea between about 0.2 m²/g and 0.5 m²/g. In some embodiments, theactive material (e.g., LFP) may have a specific surface area betweenabout 9 m²/g and 13 m²/g, or 8 m²/g and 12 m²/g. The active material mayhave a given first discharge capacity. The active material may have afirst discharge capacity of greater than or equal to about 100 milliamphours per gram (mAh/g), 105 mAh/g, 110 mAh/g, 115 mAh/g, 120 mAh/g, 125mAh/g, 130 mAh/g, 135 mAh/g, 140 mAh/g, 145 mAh/g, 150 mAh/g, 155 mAh/g,160 mAh/g, 165 mAh/g, 170 mAh/g, 175 mAh/g, 180 mAh/g, 185 mAh/g, 190mAh/g, 195 mAh/g, 200 mAh/g, 205 mAh/g, 210 mAh/g, 215 mAh/g, or 220mAh. In addition, or as an alternative, the active material may have afirst discharge capacity less than or equal to about 230 mAh/g, 225mAh/g, 220 mAh/g, 215 mAh/g, 210 mAh/g, 205 mAh/g, 200 mAh/g, 195 mAh/g,190 mAh/g, 185 mAh/g, 180 mAh/g, 175 mAh/g, 170 mAh/g, 165 mAh/g, 160mAh/g, 155 mAh/g, or 150 mAh/g. In some embodiments, the active material(e.g., NCA) may have a first discharge capacity of greater than or equalto about 195 mAh/g (e.g., at a charge/discharge rate of 0.1 C/0.1 C anda voltage window of 4.3-3.0 volts (V)). In some embodiments, the activematerial (e.g., NMC) may have a first discharge capacity greater than orequal to about 178 mAh/g (e.g., for a coin cell (e.g., CR2032) at acharge/discharge rate of 0.1 C/0.1 C and a voltage window of 3.0 V˜4.3 Vversus lithium). In some embodiments, the active material (e.g., LFP)may have a first discharge capacity of greater than or equal to about150 mAh/g (e.g., at 0.2 C). The active material may have a givencapacity. The active material may have a capacity of greater than orequal to about 80 mAh/g, 85 mAh/g, 90 mAh/g, 95 mAh/g, 100 mAh/g, 105mAh/g, 110 mAh/g, 115 mAh/g, 120 mAh/g, 125 mAh/g, 130 mAh/g, 135 mAh/g,140 mAh/g, 145 mAh/g, 150 mAh/g, 155 mAh/g, 160 mAh/g, 165 mAh/g, 170mAh/g, 175 mAh/g, 180 mAh/g, 185 mAh/g, 190 mAh/g, 195 mAh/g, 200 mAh/g,220 mAh/g, 240 mAh/g, 260 mAh/g, 280 mAh/g, 300 mAh/g, 400 mAh/g, 500mAh/g, 600 mAh/g, 700 mAh/g, 800 mAh/g, or 900 mAh/g. In addition, or asan alternative, the active material may have a capacity greater than orequal to about 600 mAh/g, 500 mAh/g, 400 mAh/g, 300 mAh/g, 250 mAh/g,210 mAh/g, 205 mAh/g, 200 mAh/g, 195 mAh/g, 190 mAh/g, 185 mAh/g, 180mAh/g, 175 mAh/g, 170 mAh/g, 165 mAh/g, 160 mAh/g, 155 mAh/g, 150 mAh/g,145 mAh/g, 140 mAh/g, 135 mAh/g, or 130 mAh/g. In some embodiments, theactive material (e.g., NMC) may have a capacity between about 162 mAh/gand 168 mAh/g (e.g., for a full cell at a charge/discharge rate of 0.5C). The active material may have a given first discharge efficiency(e.g., greater than or equal to about 75%, 81%, 82%, 83%, 84%, 85%(e.g., NMC), 86%, 87%, 88%, 89% (e.g., NCA), 90%, 91%, 92%, 93%, 94%, or95%). The active material may have any combination of one or more of theaforementioned particle size compositions, specific surface areas, firstdischarge capacities, capacities, first discharge efficiencies, andother properties.

An electrode (e.g., a positive or negative electrode of a LIB) mayinclude a binder. In some embodiments, the binder comprises at least oneof a first binder and a second binder. In some embodiments, the firstbinder is the same as the second binder. In some embodiments, the firstbinder is not the same as the second binder. A binder (e.g., a firstbinder or a second binder) may comprise, for example, one or morefluoropolymers (e.g., non-reactive thermoplastic fluoropolymers),copolymers, and/or other polymer types. Examples of binders may include,but are not limited to, polyvinyl fluoride (PVF), polyvinylidenefluoride (PVDF), polytetrafluoroethylene (PTFE),polychlorotrifluoroethylene (PCTFE), perfluoroalkoxy polymer (PFA, MFA),fluorinated ethylene-propylene (FEP), polyethylenetetrafluoroethylene(ETFE), polyethylenechlorotrifluoroethylene (ECTFE), perfluorinatedplastomer (FFPM/FFKM), fluorocarbon or (also“chlorotrifluoroethylenevinylidene fluoride” in the claims herein;FPM/FKM), fluoroelastomer (also “tetrafluoroethylene-propylene” in theclaims herein; FEPM), perfluoropolyether (PFPE), perfluorosulfonic acid(PFSA), perfluoropolyoxetane, P(VDF-trifluoroethylene),P(VDF-tetrafluoroethylene), or any combination thereof. One or more ofsuch binder materials may be present in the electrode (e.g., in thepositive electrode and/or in the negative electrode) at an individual orcombined concentration (e.g., by weight on a dry basis, without solvent)between about 0.5% and 1%, 0.5% and 2%, 0.5% and 3%, 0.5% and 4%, 0.5%and 5%, 0.5% and 6%, 0.5% and 7%, 0.5% and 8%, 0.5% and 9%, 0.5% and10%, 0.5% and 11%, 0.5% and 12%, 0.5% and 13%, 0.5% and 14%, 0.5% and15%, 0.5% and 16%, 0.5% and 17%, 0.5% and 18%, 0.5% and 19%, 0.5% and20%, 1% and 2%, 1% and 3%, 1% and 4%, 1% and 5%, 1% and 6%, 1% and 7%,1% and 8%, 1% and 9%, 1% and 10%, 1% and 11%, 1% and 12%, 1% and 13%, 1%and 14%, 1% and 15%, 1% and 16%, 1% and 17%, 1% and 18%, 1% and 19%, 1%and 20%, 2% and 3%, 2% and 4%, 2% and 5%, 2% and 6%, 2% and 7%, 2% and8%, 2% and 9%, 2% and 10%, 2% and 11%, 2% and 12%, 2% and 13%, 2% and14%, 2% and 15%, 2% and 16%, 2% and 17%, 2% and 18%, 2% and 19%, 2% and20%, 3% and 4%, 3% and 5%, 3% and 6%, 3% and 7%, 3% and 8%, 3% and 9%,3% and 10%, 3% and 11%, 3% and 12%, 3% and 13%, 3% and 14%, 3% and 15%,3% and 16%, 3% and 17%, 3% and 18%, 3% and 19%, 3% and 20%, 4% and 5%,4% and 6%, 4% and 7%, 4% and 8%, 4% and 9%, 4% and 10%, 4% and 11%, 4%and 12%, 4% and 13%, 4% and 14%, 4% and 15%, 4% and 16%, 4% and 17%, 4%and 18%, 4% and 19%, 4% and 20%, 5% and 6%, 5% and 7%, 5% and 8%, 5% and9%, 5% and 10%, 5% and 11%, 5% and 12%, 5% and 13%, 5% and 14%, 5% and15%, 5% and 16%, 5% and 17%, 5% and 18%, 5% and 19%, 5% and 20%, 6% and7%, 6% and 8%, 6% and 9%, 6% and 10%, 6% and 11%, 6% and 12%, 6% and13%, 6% and 14%, 6% and 15%, 6% and 16%, 6% and 17%, 6% and 18%, 6% and19%, 6% and 20%, 7% and 8%, 7% and 9%, 7% and 10%, 7% and 11%, 7% and12%, 7% and 13%, 7% and 14%, 7% and 15%, 7% and 16%, 7% and 17%, 7% and18%, 7% and 19%, 7% and 20%, 8% and 9%, 8% and 10%, 8% and 11%, 8% and12%, 8% and 13%, 8% and 14%, 8% and 15%, 8% and 16%, 8% and 17%, 8% and18%, 8% and 19%, 8% and 20%, 9% and 10%, 9% and 11%, 9% and 12%, 9% and13%, 9% and 14%, 9% and 15%, 9% and 16%, 9% and 17%, 9% and 18%, 9% and19%, 9% and 20%, 10% and 11%, 10% and 12%, 10% and 13%, 10% and 14%, 10%and 15%, 10% and 16%, 10% and 17%, 10% and 18%, 10% and 19%, 10% and20%, 11% and 12%, 11% and 13%, 11% and 14%, 11% and 15%, 11% and 16%,11% and 17%, 11% and 18%, 11% and 19%, 11% and 20%, 12% and 13%, 12% and14%, 12% and 15%, 12% and 16%, 12% and 17%, 12% and 18%, 12% and 19%,12% and 20%, 13% and 14%, 13% and 15%, 13% and 16%, 13% and 17%, 13% and18%, 13% and 19%, 13% and 20%, 14% and 15%, 14% and 16%, 14% and 17%,14% and 18%, 14% and 19%, 14% and 20%, 15% and 16%, 15% and 17%, 15% and18%, 15% and 19%, 15% and 20%, 16% and 17%, 16% and 18%, 16% and 19%,16% and 20%, 17% and 18%, 17% and 19%, 17% and 20%, 18% and 19%, 18% and20%, or 19% and 20%. One or more of such binder materials may be presentin the electrode (e.g., in the positive electrode and/or in the negativeelectrode) at an individual or combined concentration (e.g., by weighton a dry basis, without solvent) of greater than or equal to about 0.5%,1%, 1.5%, 2%, 2.5%, 3%, 3.5%, 4%, 4.5%, 5%, 5.5%, 6%, 6.5%, 7%, 7.5%,8%, 8.5%, 9%, 9.5%, 10%, 10.5%, 11%, 11.5%, 12%, 12.5%, 13%, 13.5%, 14%,14.5%, 15%, 15.5%, 16%, 16.5%, 17%, 17.5%, 18%, 18.5%, 19%, 19.5%, or20%. In addition, or as an alternative, one or more of such bindermaterials may be present in the electrode (e.g., in the positiveelectrode and/or in the negative electrode) at an individual or combinedconcentration of less than or equal to about 20%, 19.5%, 19%, 18.5%,18%, 17.5%, 17%, 16.5%, 16%, 15.5%, 15%, 14.5%, 14%, 13.5%, 13%, 12.5%,12%, 11.5%, 11%, 10.5%, 10%, 9.5%, 9%, 8.5%, 8%, 7.5%, 7%, 6.5%, 6%,5.5%, 5%, 4.5%, 4%, 3.5%, 3%, 2.5%, 2%, 1.5%, 1%, or 0.5%. One or moreof such binder materials may be present in the electrode at suchconcentrations in combination with one or more other materials (e.g.,one or more other electrode materials and concentrations thereofdescribed herein).

An electrode (e.g., a positive or negative electrode of a LIB) may beprepared with the aid of a solvent. A formula may include various levelsof the solvent. At least a portion or all of the solvent may evaporatefrom the electrode. Examples of solvents may include, but are notlimited to, 2-pyrrolidone (2-Py), n-vinylpyrrolidone (NVP),n-methyl-2-pyrrolidone (NMP), methyl ethyl ketone, or any combinationthereof. One or more of such solvent compounds may be present in theelectrode (e.g., in the positive electrode and/or in the negativeelectrode) at an individual or combined concentration (e.g., by weighton a wet basis) between about 20% and 25%, 20% and 30%, 20% and 35%, 20%and 40%, 20% and 45%, 20% and 50%, 20% and 55%, 20% and 60%, 20% and65%, 20% and 70%, 20% and 75%, 25% and 30%, 25% and 35%, 25% and 40%,25% and 45%, 25% and 50%, 25% and 55%, 25% and 60%, 25% and 65%, 25% and70%, 25% and 75%, 30% and 35%, 30% and 40%, 30% and 45%, 30% and 50%,30% and 55%, 30% and 60%, 30% and 65%, 30% and 70%, 30% and 75%, 35% and40%, 35% and 45%, 35% and 50%, 35% and 55%, 35% and 60%, 35% and 65%,35% and 70%, 35% and 75%, 40% and 45%, 40% and 50%, 40% and 55%, 40% and60%, 40% and 65%, 40% and 70%, 40% and 75%, 45% and 50%, 45% and 55%,45% and 60%, 45% and 65%, 45% and 70%, 45% and 75%, 50% and 55%, 50% and60%, 50% and 65%, 50% and 70%, 50% and 75%, 55% and 60%, 55% and 65%,55% and 70%, 55% and 75%, 60% and 65%, 60% and 70%, 60% and 75%, 65% and70%, 65% and 75%, or 70% and 75%. One or more of such solvent compoundsmay be present in the electrode (e.g., in the positive electrode and/orin the negative electrode) at an individual or combined concentration(e.g., by weight on a wet basis) of greater than or equal to about 20%,21%, 22%, 23%, 24%, 25%, 26%, 27%, 28%, 29%, 30%, 31%, 32%, 33%, 34%,35%, 36%, 37%, 38%, 39%, 40%, 41%, 42%, 43%, 44%, 45%, 46%, 47%, 48%,49%, 50%, 51%, 52%, 53%, 54%, 55%, 56%, 57%, 58%, 59%, 60%, 61%, 62%,63%, 64%, 65%, 66%, 67%, 68%, 69%, 70%, 71%, 72%, 73%, 74%, or 75%. Inaddition, or as an alternative, one or more of such solvent compoundsmay be present in the electrode (e.g., in the positive electrode and/orin the negative electrode) at an individual or combined concentration(e.g., by weight on a wet basis) of less than or equal to about 75%,74%, 73%, 72%, 71%, 70%, 69%, 68%, 67%, 66%, 65%, 64%, 63%, 62%, 61%,60%, 59%, 58%, 57%, 56%, 55%, 54%, 53%, 52%, 51%, 50%, 49%, 48%, 47%,46%, 45%, 44%, 43%, 42%, 41%, 40%, 39%, 38%, 37%, 36%, 35%, 34%, 33%,32%, 31%, 30%, 29%, 28%, 27%, 26%, 25%, 24%, 23%, 22%, 21%, or 20%. Oneor more of such solvent compounds may be present in the electrode atsuch concentrations in combination with one or more other materials(e.g., one or more other electrode materials and concentrations thereofdescribed herein).

An active material of an electrode (e.g., a negative electrode of a LIB)may include, for example, polyacetylene, graphite (e.g., naturalgraphite or artificial graphite), vapor-phase-grown carbon fiber, softcarbon (graphitizable carbon), hard carbon (non-graphitizable carbon),carbon nanotubes, or any combination thereof. One or more of such activematerials may be present in the electrode at an individual or combinedconcentration (e.g., by weight on a dry basis, without solvent) betweenabout 0.25% and 0.5%, 0.25% and 0.75%, 0.25% and 1%, 0.25% and 2%, 0.25%and 5%, 0.25% and 10%, 0.25% and 20%, 0.25% and 30%, 0.25% and 40%,0.25% and 50%, 0.5% and 0.75%, 0.5% and 1%, 0.5% and 2%, 0.5% and 5%,0.5% and 10%, 0.5% and 20%, 0.5% and 30%, 0.5% and 40%, 0.5% and 50%,0.75% and 1%, 0.75% and 2%, 0.75% and 5%, 0.75% and 10%, 0.75% and 20%,0.75% and 30%, 0.75% and 40%, 0.75% and 50%, 1% and 2%, 1% and 5%, 1%and 10%, 1% and 20%, 1% and 30%, 1% and 40%, 1% and 50%, 2% and 5%, 2%and 10%, 2% and 20%, 2% and 30%, 2% and 40%, 2% and 50%, 5% and 10%, 5%and 20%, 5% and 30%, 5% and 40%, 5% and 50%, 10% and 20%, 10% and 30%,10% and 40%, 10% and 50%, 20% and 30%, 20% and 40%, 20% and 50%, 30% and40%, 30% and 50%, 40% and 50%, 50% and 55%, 50% and 60%, 50% and 65%,50% and 70%, 50% and 72%, 50% and 74%, 50% and 76%, 50% and 78%, 50% and80%, 50% and 82%, 50% and 84%, 50% and 86%, 50% and 88%, 50% and 90%,50% and 91%, 50% and 92%, 50% and 93%, 50% and 94%, 50% and 95%, 50% and96%, 50% and 97%, 50% and 98%, 50% and 99%, 55% and 60%, 55% and 65%,55% and 70%, 55% and 72%, 55% and 74%, 55% and 76%, 55% and 78%, 55% and80%, 55% and 82%, 55% and 84%, 55% and 86%, 55% and 88%, 55% and 90%,55% and 91%, 55% and 92%, 55% and 93%, 55% and 94%, 55% and 95%, 55% and96%, 55% and 97%, 55% and 98%, 55% and 99%, 60% and 65%, 60% and 70%,60% and 72%, 60% and 74%, 60% and 76%, 60% and 78%, 60% and 80%, 60% and82%, 60% and 84%, 60% and 86%, 60% and 88%, 60% and 90%, 60% and 91%,60% and 92%, 60% and 93%, 60% and 94%, 60% and 95%, 60% and 96%, 60% and97%, 60% and 98%, 60% and 99%, 65% and 70%, 65% and 72%, 65% and 74%,65% and 76%, 65% and 78%, 65% and 80%, 65% and 82%, 65% and 84%, 65% and86%, 65% and 88%, 65% and 90%, 65% and 91%, 65% and 92%, 65% and 93%,65% and 94%, 65% and 95%, 65% and 96%, 65% and 97%, 65% and 98%, 65% and99%, 70% and 72%, 70% and 74%, 70% and 76%, 70% and 78%, 70% and 80%,70% and 82%, 70% and 84%, 70% and 86%, 70% and 88%, 70% and 90%, 70% and91%, 70% and 92%, 70% and 93%, 70% and 94%, 70% and 95%, 70% and 96%,70% and 97%, 70% and 98%, 70% and 99%, 72% and 74%, 72% and 76%, 72% and78%, 72% and 80%, 72% and 82%, 72% and 84%, 72% and 86%, 72% and 88%,72% and 90%, 72% and 91%, 72% and 92%, 72% and 93%, 72% and 94%, 72% and95%, 72% and 96%, 72% and 97%, 72% and 98%, 72% and 99%, 74% and 76%,74% and 78%, 74% and 80%, 74% and 82%, 74% and 84%, 74% and 86%, 74% and88%, 74% and 90%, 74% and 91%, 74% and 92%, 74% and 93%, 74% and 94%,74% and 95%, 74% and 96%, 74% and 97%, 74% and 98%, 74% and 99%, 76% and78%, 76% and 80%, 76% and 82%, 76% and 84%, 76% and 86%, 76% and 88%,76% and 90%, 76% and 91%, 76% and 92%, 76% and 93%, 76% and 94%, 76% and95%, 76% and 96%, 76% and 97%, 76% and 98%, 76% and 99%, 78% and 80%,78% and 82%, 78% and 84%, 78% and 86%, 78% and 88%, 78% and 90%, 78% and91%, 78% and 92%, 78% and 93%, 78% and 94%, 78% and 95%, 78% and 96%,78% and 97%, 78% and 98%, 78% and 99%, 80% and 82%, 80% and 84%, 80% and86%, 80% and 88%, 80% and 90%, 80% and 91%, 80% and 92%, 80% and 93%,80% and 94%, 80% and 95%, 80% and 96%, 80% and 97%, 80% and 98%, 80% and99%, 82% and 84%, 82% and 86%, 82% and 88%, 82% and 90%, 82% and 91%,82% and 92%, 82% and 93%, 82% and 94%, 82% and 95%, 82% and 96%, 82% and97%, 82% and 98%, 82% and 99%, 84% and 86%, 84% and 88%, 84% and 90%,84% and 91%, 84% and 92%, 84% and 93%, 84% and 94%, 84% and 95%, 84% and96%, 84% and 97%, 84% and 98%, 84% and 99%, 86% and 88%, 86% and 90%,86% and 91%, 86% and 92%, 86% and 93%, 86% and 94%, 86% and 95%, 86% and96%, 86% and 97%, 86% and 98%, 86% and 99%, 88% and 90%, 88% and 91%,88% and 92%, 88% and 93%, 88% and 94%, 88% and 95%, 88% and 96%, 88% and97%, 88% and 98%, 88% and 99%, 90% and 91%, 90% and 92%, 90% and 93%,90% and 94%, 90% and 95%, 90% and 96%, 90% and 97%, 90% and 98%, 90% and99%, 91% and 92%, 91% and 93%, 91% and 94%, 91% and 95%, 91% and 96%,91% and 97%, 91% and 98%, 91% and 99%, 92% and 93%, 92% and 94%, 92% and95%, 92% and 96%, 92% and 97%, 92% and 98%, 92% and 99%, 93% and 94%,93% and 95%, 93% and 96%, 93% and 97%, 93% and 98%, 93% and 99%, 94% and95%, 94% and 96%, 94% and 97%, 94% and 98%, 94% and 99%, 95% and 96%,95% and 97%, 95% and 98%, 95% and 99%, 96% and 97%, 96% and 98%, 96% and99%, 97% and 98%, 97% and 99%, or 98% and 99%. One or more of suchactive materials may be present in the electrode at an individual orcombined concentration (e.g., by weight on a dry basis, without solvent)of greater than or equal to about 50%, 51%, 52%, 53%, 54%, 55%, 56%,57%, 58%, 59%, 60%, 61%, 62%, 63%, 64%, 65%, 66%, 67%, 68%, 69%, 70%,70.5%, 71%, 71.5%, 72%, 72.5%, 73%, 73.5%, 74%, 74.5%, 75%, 75.5%, 76%,76.5%, 77%, 77.5%, 78%, 78.5%, 79%, 79.5%, 80%, 80.5%, 81%, 81.5%, 82%,82.5%, 83%, 83.5%, 84%, 84.5%, 85%, 85.5%, 86%, 86.5%, 87%, 87.5%, 88%,88.5%, 89%, 89.5%, 90%, 90.5%, 91%, 91.5%, 92%, 92.5%, 93%, 93.5%, 94%,94.5%, 95%, 95.5%, 96%, 96.5%, 97%, 97.5%, 98%, 98.5%, 99%, or 99.5%. Inaddition, or as an alternative, one or more of such active materials maybe present in the electrode at an individual or combined concentration(e.g., by weight on a dry basis, without solvent) of less than or equalto about 99.5%, 99%, 98.5%, 98%, 97.5%, 97%, 96.5%, 96%, 95.5%, 95%,94.5%, 94%, 93.5%, 93%, 92.5%, 92%, 91.5%, 91%, 90.5%, 90%, 89.5%, 89%,88.5%, 88%, 87.5%, 87%, 86.5%, 86%, 85.5%, 85%, 84.5%, 84%, 83.5%, 83%,82.5%, 82%, 81.5%, 81%, 80.5%, 80%, 79.5%, 79%, 78.5%, 78%, 77.5%, 77%,76.5%, 76%, 75.5%, 75%, 74.5%, 74%, 73.5%, 73%, 72.5%, 72%, 71.5%, 71%,70.5%, 70%, 69%, 68%, 67%, 66%, 65%, 64%, 63%, 62%, 61%, 60%, 59%, 58%,57%, 56%, 55%, 54%, 53%, 52%, 51%, or 50%. One or more of such activematerials may be present in the electrode at such concentrations incombination with one or more other materials (e.g., one or more otherelectrode materials and concentrations thereof described herein).

The aforementioned active material may have a particle size distributionsuch that, for example, 10% of the particles are smaller than about 11μm, 10 μm, 9 μm, 8 μm, 7 μm, 6 μm, 5 μm, or 4 μm. The active materialmay have such particle size distribution in combination with, forexample, 50% of the particles being smaller than about 16 μm, 15 μm, 14μm, 13 μm, 12 μm, 11 μm, 10 μm, or 9 μm. The active material may suchparticle size distribution in combination with, for example, 90% of theparticles being smaller than about 31 μm, 30 μm, 29 μm, 28 μm, 27 μm, 26μm, 25 μm, 24 μm, 23 μm, 22 μm, 21 μm, 20 μm, 19 μm, 18 μm, 17 μm, 16μm, 15 μm, or 14 μm. In one embodiment, the active material may have aparticle size distribution characterized by 10% of the particles smallerthan about 6.8 μm, 50% of the particles smaller than about 11.6 μm and90% of the particles smaller than about 19.3 μm. The active material mayhave a given tap density (e.g., a tap density of less than or equal toabout 1.5 grams per cubic centimeter (g/cm³), 1.4 g/cm³, 1.3 g/cm³, 1.2g/cm³, 1.1 g/cm³, 1 g/cm³, 0.9 g/cm³, 0.8 g/cm³, 0.7 g/cm³, 0.6 g/cm³,or 0.5 g/cm³). In one embodiment, the active material may have a tapdensity of less than or equal to about 0.99 g/cm³. The active materialmay have a given specific surface area (e.g., greater than or equal toabout 1 m²/g, 1.5 m²/g, 2 m²/g, 2.5 m²/g, 3 m²/g, 3.5 m²/g, 4 m²/g, 4.5m²/g, 5 m²/g, 5.5 m²/g, 6 m²/g, 6.5 m²/g, or 7 m²/g). In one embodiment,the active material may have a specific surface area of at least about3.8 m²/g. The active material may have a given first capacity or firstdischarge capacity. The active material may have a first capacity orfirst discharge capacity of at least about 320 mAh/g, 325 mAh/g, 330mAh/g, 335 mAh/g, 340 mAh/g, 345 mAh/g, 350 mAh/g, 351 mAh/g, 352 mAh/g,353 mAh/g, 354 mAh/g, 355 mAh/g, 356 mAh/g, 357 mAh/g, 358 mAh/g, 359mAh/g, 360 mAh/g, 361 mAh/g, 362 mAh/g, 363 mAh/g, 364 mAh/g, 365 mAh/g,366 mAh/g, 367 mAh/g, 368 mAh/g, 369 mAh/g, 370 mAh/g, 371 mAh/g, 372mAh/g, 373 mAh/g, 374 mAh/g, 375 mAh/g, 376 mAh/g, 377 mAh/g, 378 mAh/g,379 mAh/g, 380 mAh/g, 385 mAh/g, 390 mAh/g, 395 mAh/g or 400 mAh/g. Inone embodiment, the active material may have a first capacity of atleast about 364.9 mAh/g. The active material may have a given efficiencyor first discharge efficiency. The active material may have anefficiency or first discharge efficiency of at least about 80%, 81%,82%, 83%, 84%, 85%, 86%, 87%, 88%, 89%, 90%, 91%, 91.5%, 92%, 92.5%,93%, 93.5%, 94%, 94.5%, 95%, 95.5%, 96%, 96.5%, 97%, 97.5%, 98%, 98.5%,or 99%. In one embodiment, the active material may have an efficiency ofat least about 94.5%. The active material may have a given wettability(e.g., a time to wet surface of at least about 80 seconds (s), 82 s, 84s, 86 s, 88 s, 90 s, 92 s, 94 s, 96 s, 98 s, 100 s, 105 s, 110 s, or 115s). In one embodiment, the active material may have a wettability of atleast about 92 s. The active material may have a given powderconductivity (e.g., at least about 250 siemens per centimeter (S/cm),255 S/cm, 260 S/cm, 265 S/cm, 270 S/cm, 275 S/cm, 280 S/cm, 285 S/cm,290 S/cm, 295 S/cm, 300 S/cm, 305 S/cm, 310 S/cm, 315 S/cm, 320 S/cm,325 S/cm, 330 S/cm, 335 S/cm, 340 S/cm, 345 S/cm, 350 S/cm, 355 S/cm,360 S/cm, 365 S/cm or 370 S/cm). In one embodiment, the active materialmay have a powder conductivity of at least about 340 S/cm. The activematerial may have a given crystal orientation. The active material mayhave any combination of one or more of the aforementioned particle sizedistributions, tap densities, specific surface areas, pellet densities,first capacities, efficiencies, or first discharge efficiencies,wettability, powder conductivities, and other properties (e.g., crystalorientations).

An electrode (e.g., a negative electrode of a LIB) may includeconductive additive(s). A conductive additive may comprise, for example,conductive carbon. Examples of conductive additives may include, but arenot limited to, carbon black (e.g., acetylene black, furnace black, orother carbon types), vapor-grown carbon fibers, carbon nanotubes, or anycombination thereof. One or more of such conductive additives may bepresent in the electrode at an individual or combined concentration(e.g., by weight on a dry basis, without solvent) between about 0.1% and0.5%, 0.1% and 1%, 0.1% and 1.5%, 0.1% and 2%, 0.1% and 2.5%, 0.1% and3%, 0.1% and 3.5%, 0.1% and 4%, 0.1% and 4.5%, 0.1% and 5%, 0.1% and5.5%, 0.1% and 6%, 0.1% and 6.5%, 0.1% and 7%, 0.1% and 7.5%, 0.1% and8%, 0.1% and 8.5%, 0.1% and 9%, 0.1% and 9.5%, 0.1% and 10%, 0.5% and1%, 0.5% and 1.5%, 0.5% and 2%, 0.5% and 2.5%, 0.5% and 3%, 0.5% and3.5%, 0.5% and 4%, 0.5% and 4.5%, 0.5% and 5%, 0.5% and 5.5%, 0.5% and6%, 0.5% and 6.5%, 0.5% and 7%, 0.5% and 7.5%, 0.5% and 8%, 0.5% and8.5%, 0.5% and 9%, 0.5% and 9.5%, 0.5% and 10%, 1% and 1.5%, 1% and 2%,1% and 2.5%, 1% and 3%, 1% and 3.5%, 1% and 4%, 1% and 4.5%, 1% and 5%,1% and 5.5%, 1% and 6%, 1% and 6.5%, 1% and 7%, 1% and 7.5%, 1% and 8%,1% and 8.5%, 1% and 9%, 1% and 9.5%, 1% and 10%, 1.5% and 2%, 1.5% and2.5%, 1.5% and 3%, 1.5% and 3.5%, 1.5% and 4%, 1.5% and 4.5%, 1.5% and5%, 1.5% and 5.5%, 1.5% and 6%, 1.5% and 6.5%, 1.5% and 7%, 1.5% and7.5%, 1.5% and 8%, 1.5% and 8.5%, 1.5% and 9%, 1.5% and 9.5%, 1.5% and10%, 2% and 2.5%, 2% and 3%, 2% and 3.5%, 2% and 4%, 2% and 4.5%, 2% and5%, 2% and 5.5%, 2% and 6%, 2% and 6.5%, 2% and 7%, 2% and 7.5%, 2% and8%, 2% and 8.5%, 2% and 9%, 2% and 9.5%, 2% and 10%, 2.5% and 3%, 2.5%and 3.5%, 2.5% and 4%, 2.5% and 4.5%, 2.5% and 5%, 2.5% and 5.5%, 2.5%and 6%, 2.5% and 6.5%, 2.5% and 7%, 2.5% and 7.5%, 2.5% and 8%, 2.5% and8.5%, 2.5% and 9%, 2.5% and 9.5%, 2.5% and 10%, 3% and 3.5%, 3% and 4%,3% and 4.5%, 3% and 5%, 3% and 5.5%, 3% and 6%, 3% and 6.5%, 3% and 7%,3% and 7.5%, 3% and 8%, 3% and 8.5%, 3% and 9%, 3% and 9.5%, 3% and 10%,3.5% and 4%, 3.5% and 4.5%, 3.5% and 5%, 3.5% and 5.5%, 3.5% and 6%,3.5% and 6.5%, 3.5% and 7%, 3.5% and 7.5%, 3.5% and 8%, 3.5% and 8.5%,3.5% and 9%, 3.5% and 9.5%, 3.5% and 10%, 4% and 4.5%, 4% and 5%, 4% and5.5%, 4% and 6%, 4% and 6.5%, 4% and 7%, 4% and 7.5%, 4% and 8%, 4% and8.5%, 4% and 9%, 4% and 9.5%, 4% and 10%, 4.5% and 5%, 4.5% and 5.5%,4.5% and 6%, 4.5% and 6.5%, 4.5% and 7%, 4.5% and 7.5%, 4.5% and 8%,4.5% and 8.5%, 4.5% and 9%, 4.5% and 9.5%, 4.5% and 10%, 5% and 5.5%, 5%and 6%, 5% and 6.5%, 5% and 7%, 5% and 7.5%, 5% and 8%, 5% and 8.5%, 5%and 9%, 5% and 9.5%, 5% and 10%, 5.5% and 6%, 5.5% and 6.5%, 5.5% and7%, 5.5% and 7.5%, 5.5% and 8%, 5.5% and 8.5%, 5.5% and 9%, 5.5% and9.5%, 5.5% and 10%, 6% and 6.5%, 6% and 7%, 6% and 7.5%, 6% and 8%, 6%and 8.5%, 6% and 9%, 6% and 9.5%, 6% and 10%, 6.5% and 7%, 6.5% and7.5%, 6.5% and 8%, 6.5% and 8.5%, 6.5% and 9%, 6.5% and 9.5%, 6.5% and10%, 7% and 7.5%, 7% and 8%, 7% and 8.5%, 7% and 9%, 7% and 9.5%, 7% and10%, 7.5% and 8%, 7.5% and 8.5%, 7.5% and 9%, 7.5% and 9.5%, 7.5% and10%, 8% and 8.5%, 8% and 9%, 8% and 9.5%, 8% and 10%, 8.5% and 9%, 8.5%and 9.5%, 8.5% and 10%, 9% and 9.5%, 9% and 10%, or 9.5% and 10%. One ormore of such conductive additives may be present in the electrode at anindividual or combined concentration (e.g., by weight on a dry basis,without solvent) of greater than or equal to about 0.1%, 0.5%, 1%, 1.5%,2%, 2.5%, 3%, 3.5%, 4%, 4.5%, 5%, 5.5%, 6%, 6.5%, 7%, 7.5%, 8%, 8.5%,9%, 9.5%, or 10%. In addition, or as an alternative, one or more of suchconductive additives may be present in the electrode at an individual orcombined concentration (e.g., by weight on a dry basis, without solvent)of less than or equal to about 10%, 9.5%, 9%, 8.5%, 8%, 7.5%, 7%, 6.5%,6%, 5.5%, 5%, 4.5%, 4%, 3.5%, 3%, 2.5%, 2%, 1.5%, 1%, 0.5%, or 0.1%. Oneor more of such conductive additives may be present in the electrode atsuch concentrations in combination with one or more other materials(e.g., one or more other electrode materials and concentrations thereofdescribed herein).

The aforementioned conductive additive may have a given conductivity.The conductive additive may have an electrical conductivity of at leastabout 5 S/cm, 6 S/cm, 7 S/cm, 8 S/cm, 9 S/cm, 10 S/cm, 15 S/cm, 20 S/cm,30 S/cm, 35 S/cm, 40 S/cm, 45 S/cm, 50 S/cm, 55 S/cm, 60 S/cm, or 65S/cm. The conductive additive may be a powder. In some embodiments, thepowder may initially be compressed (e.g., 50% or 100% compressed). Theconductive additive may have a given surface area. The conductiveadditive may have a surface area (e.g., Brunauer, Emmett and Teller(BET) nitrogen surface area, as measured, for example, by ASTM D3037-89test method) of at least about 10 m²/g, 15 m²/g, 20 m²/g, 25 m²/g, 30m²/g, 35 m²/g, 40 m²/g, 45 m²/g, 50 m²/g, 55 m²/g, 60 m²/g, 65 m²/g, or70 m²/g. The conductive additive may have a given density. Theconductive additive may have a density (e.g., in the bag, as measured bya suitable test method) of at least about 100 kilograms per cubic meter(kg/m³), 110 kg/m³, 120 kg/m³, 130 kg/m³, 140 kg/m³, 150 kg/m³, 160kg/m³, 170 kg/m³, 180 kg/m³, 200 kg/m³, 210 kg/m³, 220 kg/m³, 230 kg/m³,240 kg/m³, or 250 kg/m³.

The carbon-based material of the present disclosure may be used in anelectrode as active material, as conductive additive, and/or as binder.In certain embodiments, use of the carbon-based material of the presentdisclosure in an electrode may allow improved utilization of activematerial(s) in the electrode. For example, in a conventional LIB, asignificant portion of the electrode may not be active, as a largeamount of conductive additive (e.g., carbon black) may need to be addedto allow the percolation threshold to be reached. In an example, apercolation threshold of carbon black in positive electrodes oflithium-ion batteries (e.g., in LFP) is about 10-15 wt %. A large amountof conductive additive (e.g., about 10-15 wt % carbon black) maytherefore need to be added to the electrode to reach the percolationthreshold, thereby decreasing the amount of active material that may beprovided. The threshold value may depend on the size and aspect ratio ofparticles in the active material of the positive electrode (e.g., metaloxide may form spherical particles with a diameter of between about 2microns and 10 microns). When the carbon-based material of the presentdisclosure is used instead of carbon black (or other conductiveadditives), the percolation threshold may be significantly lowered(e.g., by a factor of at least about 2, 3, 4, 5, or more). Suchdecreases in the percolation threshold may be achieved when thecarbon-based material is used alone or in combination with one or moreother conductive additives (e.g., in combination with some of theconductive additives that it replaces). The carbon-based material of thepresent disclosure may be used to entirely replace other conductiveadditives. In such a case, a percolation threshold may or may not exist.Use of the carbon-based material of the present disclosure (alone or incombination with one or more other conductive additives) may allow atleast about 5%, 10%, 15%, 20%, or 25% (e.g., by weight) more activematerial to be incorporated in the electrode when compared with anelectrode with substantially the same conductivity (e.g., electricalconductivity) that does not comprise the present carbon-based material.The improved performance of the carbon-based network described hereinmay result from its composition, morphology, and/or distribution. Forexample, the carbon-based material may have a higher conductivity perunit weight. The carbon-based material may have a higher conductivityper unit weight serve as binder. In some embodiments, as describedelsewhere herein, the carbon-based material described herein may formPCS. The carbon in the carbon-based material of the present disclosuremay form a porous network. At least a portion of the carbon-basedmaterial of the present disclosure may comprise non-sp2 carbon.

A carbon-based material of the present disclosure (e.g., PCS) may bepresent in an electrode (e.g., a positive electrode of a LIB) at aconcentration (e.g., by weight on a dry basis, without solvent) betweenabout 0.01% and 0.05%, 0.01% and 0.1%, 0.01% and 0.5%, 0.01% and 1%,0.01% and 2%, 0.01% and 3%, 0.01% and 4%, 0.01% and 5%, 0.01% and 6%,0.01% and 7%, 0.01% and 8%, 0.01% and 9%, 0.01% and 10%, 0.01% and 11%,0.01% and 12%, 0.01% and 13%, 0.01% and 14%, 0.01% and 15%, 0.01% and16%, 0.01% and 17%, 0.01% and 18%, 0.01% and 19%, 0.01% and 20%, 0.01%and 25%, 0.01% and 30%, 0.01% and 35%, 0.01% and 40%, 0.05% and 0.1%,0.05% and 0.5%, 0.05% and 1%, 0.05% and 2%, 0.05% and 3%, 0.05% and 4%,0.05% and 5%, 0.05% and 6%, 0.05% and 7%, 0.05% and 8%, 0.05% and 9%,0.05% and 10%, 0.05% and 11%, 0.05% and 12%, 0.05% and 13%, 0.05% and14%, 0.05% and 15%, 0.05% and 16%, 0.05% and 17%, 0.05% and 18%, 0.05%and 19%, 0.05% and 20%, 0.05% and 25%, 0.05% and 30%, 0.05% and 35%,0.05% and 40%, 0.1% and 0.5%, 0.1% and 1%, 0.1% and 2%, 0.1% and 3%,0.1% and 4%, 0.1% and 5%, 0.1% and 6%, 0.1% and 7%, 0.1% and 8%, 0.1%and 9%, 0.1% and 10%, 0.1% and 11%, 0.1% and 12%, 0.1% and 13%, 0.1% and14%, 0.1% and 15%, 0.1% and 16%, 0.1% and 17%, 0.1% and 18%, 0.1% and19%, 0.1% and 20%, 0.1% and 25%, 0.1% and 30%, 0.1% and 35%, 0.1% and40%, 0.5% and 1%, 0.5% and 2%, 0.5% and 3%, 0.5% and 4%, 0.5% and 5%,0.5% and 6%, 0.5% and 7%, 0.5% and 8%, 0.5% and 9%, 0.5% and 10%, 0.5%and 11%, 0.5% and 12%, 0.5% and 13%, 0.5% and 14%, 0.5% and 15%, 0.5%and 16%, 0.5% and 17%, 0.5% and 18%, 0.5% and 19%, 0.5% and 20%, 0.5%and 25%, 0.5% and 30%, 0.5% and 35%, 0.5% and 40%, 1% and 2%, 1% and 3%,1% and 4%, 1% and 5%, 1% and 6%, 1% and 7%, 1% and 8%, 1% and 9%, 1% and10%, 1% and 11%, 1% and 12%, 1% and 13%, 1% and 14%, 1% and 15%, 1% and16%, 1% and 17%, 1% and 18%, 1% and 19%, 1% and 20%, 1% and 25%, 1% and30%, 1% and 35%, 1% and 40%, 2% and 3%, 2% and 4%, 2% and 5%, 2% and 6%,2% and 7%, 2% and 8%, 2% and 9%, 2% and 10%, 2% and 11%, 2% and 12%, 2%and 13%, 2% and 14%, 2% and 15%, 2% and 16%, 2% and 17%, 2% and 18%, 2%and 19%, 2% and 20%, 2% and 25%, 2% and 30%, 2% and 35%, 2% and 40%, 3%and 4%, 3% and 5%, 3% and 6%, 3% and 7%, 3% and 8%, 3% and 9%, 3% and10%, 3% and 11%, 3% and 12%, 3% and 13%, 3% and 14%, 3% and 15%, 3% and16%, 3% and 17%, 3% and 18%, 3% and 19%, 3% and 20%, 3% and 25%, 3% and30%, 3% and 35%, 3% and 40%, 4% and 5%, 4% and 6%, 4% and 7%, 4% and 8%,4% and 9%, 4% and 10%, 4% and 11%, 4% and 12%, 4% and 13%, 4% and 14%,4% and 15%, 4% and 16%, 4% and 17%, 4% and 18%, 4% and 19%, 4% and 20%,4% and 25%, 4% and 30%, 4% and 35%, 4% and 40%, 5% and 6%, 5% and 7%, 5%and 8%, 5% and 9%, 5% and 10%, 5% and 11%, 5% and 12%, 5% and 13%, 5%and 14%, 5% and 15%, 5% and 16%, 5% and 17%, 5% and 18%, 5% and 19%, 5%and 20%, 5% and 25%, 5% and 30%, 5% and 35%, 5% and 40%, 6% and 7%, 6%and 8%, 6% and 9%, 6% and 10%, 6% and 11%, 6% and 12%, 6% and 13%, 6%and 14%, 6% and 15%, 6% and 16%, 6% and 17%, 6% and 18%, 6% and 19%, 6%and 20%, 6% and 25%, 6% and 30%, 6% and 35%, 6% and 40%, 7% and 8%, 7%and 9%, 7% and 10%, 7% and 11%, 7% and 12%, 7% and 13%, 7% and 14%, 7%and 15%, 7% and 16%, 7% and 17%, 7% and 18%, 7% and 19%, 7% and 20%, 7%and 25%, 7% and 30%, 7% and 35%, 7% and 40%, 8% and 9%, 8% and 10%, 8%and 11%, 8% and 12%, 8% and 13%, 8% and 14%, 8% and 15%, 8% and 16%, 8%and 17%, 8% and 18%, 8% and 19%, 8% and 20%, 8% and 25%, 8% and 30%, 8%and 35%, 8% and 40%, 9% and 10%, 9% and 11%, 9% and 12%, 9% and 13%, 9%and 14%, 9% and 15%, 9% and 16%, 9% and 17%, 9% and 18%, 9% and 19%, 9%and 20%, 9% and 25%, 9% and 30%, 9% and 35%, 9% and 40%, 10% and 11%,10% and 12%, 10% and 13%, 10% and 14%, 10% and 15%, 10% and 16%, 10% and17%, 10% and 18%, 10% and 19%, 10% and 20%, 10% and 25%, 10% and 30%,10% and 35%, 10% and 40%, 11% and 12%, 11% and 13%, 11% and 14%, 11% and15%, 11% and 16%, 11% and 17%, 11% and 18%, 11% and 19%, 11% and 20%,11% and 25%, 11% and 30%, 11% and 35%, 11% and 40%, 12% and 13%, 12% and14%, 12% and 15%, 12% and 16%, 12% and 17%, 12% and 18%, 12% and 19%,12% and 20%, 12% and 25%, 12% and 30%, 12% and 35%, 12% and 40%, 13% and14%, 13% and 15%, 13% and 16%, 13% and 17%, 13% and 18%, 13% and 19%,13% and 20%, 13% and 25%, 13% and 30%, 13% and 35%, 13% and 40%, 14% and15%, 14% and 16%, 14% and 17%, 14% and 18%, 14% and 19%, 14% and 20%,14% and 25%, 14% and 30%, 14% and 35%, 14% and 40%, 15% and 16%, 15% and17%, 15% and 18%, 15% and 19%, 15% and 20%, 15% and 25%, 15% and 30%,15% and 35%, 15% and 40%, 16% and 17%, 16% and 18%, 16% and 19%, 16% and20%, 16% and 25%, 16% and 30%, 16% and 35%, 16% and 40%, 17% and 18%,17% and 19%, 17% and 20%, 17% and 25%, 17% and 30%, 17% and 35%, 17% and40%, 18% and 19%, 18% and 20%, 18% and 25%, 18% and 30%, 18% and 35%,18% and 40%, 19% and 20%, 19% and 25%, 19% and 30%, 19% and 35%, 19% and40%, 20% and 25%, 20% and 30%, 20% and 35%, 20% and 40%, 25% and 30%,25% and 35%, 25% and 40%, 30% and 35%, 30% and 40%, or 35% and 40%. Thecarbon-based material may be present in the electrode at a concentration(e.g., by weight on a dry basis, without solvent) of greater than orequal to about 0.01%, 0.05%, 0.1%, 0.5%, 1%, 1.5%, 2%, 2.5%, 3%, 3.5%,4%, 4.5%, 5%, 5.5%, 6%, 6.5%, 7%, 7.5%, 8%, 8.5%, 9%, 9.5%, 10%, 10.5%,11%, 11.5%, 12%, 12.5%, 13%, 13.5%, 14%, 14.5%, 15%, 15.5%, 16%, 16.5%,17%, 17.5%, 18%, 18.5%, 19%, 19.5%, 20%, 21%, 22%, 23%, 24%, 25%, 26%,27%, 28%, 29%, 30%, 31%, 32%, 33%, 34%, 35%, 36%, 37%, 38%, 39%, or 40%.In addition, or as an alternative, the carbon-based material may bepresent in the electrode at a concentration (e.g., by weight on a drybasis, without solvent) of less than or equal to about 40%, 39%, 38%,37%, 36%, 35%, 34%, 33%, 32%, 31%, 30%, 29%, 28%, 27%, 26%, 25%, 24%,23%, 22%, 21%, 20%, 19.5%, 19%, 18.5%, 18%, 17.5%, 17%, 16.5%, 16%,15.5%, 15%, 14.5%, 14%, 13.5%, 13%, 12.5%, 12%, 11.5%, 11%, 10.5%, 10%,9.5%, 9%, 8.5%, 8%, 7.5%, 7%, 6.5%, 6%, 5.5%, 5%, 4.5%, 4%, 3.5%, 3%,2.5%, 2%, 1.5%, 1%, 0.5%, 0.1%, 0.05%, or 0.01%. The carbon-basedmaterial may be present in the electrode at such concentrations incombination with one or more other materials (e.g., one or more otherelectrode materials and concentrations thereof described herein).

In certain embodiments, the carbon-based material of the presentdisclosure (e.g., PCS) may be present in an electrode (e.g., anelectrode of a supercapacitor) at a concentration (e.g., by weight) ofgreater than or equal to about 0.01%, 0.05%, 0.1%, 0.5%, 1%, 1.5%, 2%,2.5%, 3%, 3.5%, 4%, 4.5%, 5%, 5.5%, 6%, 6.5%, 7%, 7.5%, 8%, 8.5%, 9%,9.5%, 10%, 10.5%, 11%, 11.5%, 12%, 12.5%, 13%, 13.5%, 14%, 14.5%, 15%,15.5%, 16%, 16.5%, 17%, 17.5%, 18%, 18.5%, 19%, 19.5%, 20%, 25%, 30%,35%, 40%, 45%, 50%, 60%, 65%, 70%, 75%, 80%, 85%, 90%, or 95%.

Methods of Forming Energy Storage Devices

An energy storage device of the present disclosure may compriseelectrodes, separator(s), electrolyte, and packaging. Such componentsmay be fabricated and assembled in different ways. In certainembodiments, individual components may be fabricated and laterassembled. In some embodiments, the components may be assembled throughwinding or rolling (e.g., see FIG. 9 and FIG. 20). For example, a methodof making a battery cell may comprise providing a first sheet of aseparator, placing a positive electrode sheet (e.g., comprising acarbon-based material of the present disclosure) on the first sheet ofseparator, placing a second sheet of the separator on the positiveelectrode sheet, placing a negative electrode sheet (e.g., comprisinggraphite) on the second sheet of the separator, and rolling the sheetsto form the battery cell (a rolled cell). In some embodiments, thecomponents may be assembled through stacking (e.g., see FIG. 18 and FIG.19).

FIG. 2 schematically illustrates an example of a process of getting aformula and processing of a battery comprising a carbon-based materialof the present disclosure. The formula may include at least a portion ofan electrode mixture (e.g., a cathode mixture). In certain embodiments,a formula may include all components of an electrode mixture (e.g., thewhole cathode mixture). In certain embodiments, the formula may be ormay form a slurry. The process may include providing a binder 201 and asolvent 202. The binder 201 and the solvent 202 may be combined in areactor 203. The reactor 203 may be heated to a given temperature (e.g.,at least about 90° C.). The process may include providing a lithiatedmetal compound (e.g., lithiated metal oxide or phosphate) 204 and thecarbon-based material (e.g., PCS) 205. A mixer 206 may receive at leasta portion of the material from the reactor 203 (e.g., heated binder andheated solvent), the lithiated metal compound (e.g., lithiated metaloxide or phosphate) 204 and the carbon-based material (e.g., PCS) 205.The mixer 206 may output a slurry 207 (e.g., comprising a mixture of thecomponents in the mixer). The slurry 207 may be processed through rollcoating and drying 208, followed by a roll press 210. Then, the processmay comprise slitting 211 and application of metal tabs 212. The processmay further comprise winding 213, followed by necking 214. The processmay further include electrolyte addition 215. Finally, the process mayinclude cell crimping 216.

Alternatively, in some embodiments, at least a portion of the binder201, solvent 202, lithiated metal compound 204, carbon-based material205, and/or any other electrode components may be otherwise combined.For example, these components or a subset thereof may all be provideddirectly to the mixer 206 (e.g., which may be heated).

FIG. 25 illustratively depicts an exemplary apparatus for roll coating,wherein a slot die 2501 deposits a slurry 2502 on a film 2503, as thefilm 2503 passes over a roller 2504.

FIGS. 3-7 show examples of processing of battery electrode(s). Suchprocessing may include one or more process(ing) steps (e.g., step 208 inFIG. 2). The process(ing) may include coating of a substrate with aslurry (e.g., a slurry comprising the carbon-based material, forexample, PCS) using large scale roll-to-roll processing as shown in FIG.3. The substrate (e.g., if conductive) may serve as an electrode currentcollector. In some embodiments, the process(ing) may include using analuminum foil as a substrate. The aluminum foil may form a currentcollector.

In some embodiments, the active material is present in the slurry at aconcentration of about 20% to about 75%. In some embodiments, the activematerial is present in the slurry at a concentration of at least about20%. In some embodiments, the active material is present in the slurryat a concentration of at most about 75%. In some embodiments, the activematerial is present in the slurry at a concentration of about 20% toabout 25%, about 20% to about 30%, about 20% to about 35%, about 20% toabout 40%, about 20% to about 45%, about 20% to about 50%, about 20% toabout 55%, about 20% to about 60%, about 20% to about 65%, about 20% toabout 70%, about 20% to about 75%, about 25% to about 30%, about 25% toabout 35%, about 25% to about 40%, about 25% to about 45%, about 25% toabout 50%, about 25% to about 55%, about 25% to about 60%, about 25% toabout 65%, about 25% to about 70%, about 25% to about 75%, about 30% toabout 35%, about 30% to about 40%, about 30% to about 45%, about 30% toabout 50%, about 30% to about 55%, about 30% to about 60%, about 30% toabout 65%, about 30% to about 70%, about 30% to about 75%, about 35% toabout 40%, about 35% to about 45%, about 35% to about 50%, about 35% toabout 55%, about 35% to about 60%, about 35% to about 65%, about 35% toabout 70%, about 35% to about 75%, about 40% to about 45%, about 40% toabout 50%, about 40% to about 55%, about 40% to about 60%, about 40% toabout 65%, about 40% to about 70%, about 40% to about 75%, about 45% toabout 50%, about 45% to about 55%, about 45% to about 60%, about 45% toabout 65%, about 45% to about 70%, about 45% to about 75%, about 50% toabout 55%, about 50% to about 60%, about 50% to about 65%, about 50% toabout 70%, about 50% to about 75%, about 55% to about 60%, about 55% toabout 65%, about 55% to about 70%, about 55% to about 75%, about 60% toabout 65%, about 60% to about 70%, about 60% to about 75%, about 65% toabout 70%, about 65% to about 75%, or about 70% to about 75%. In someembodiments, the active material is present in the slurry at aconcentration of about 20%, about 25%, about 30%, about 35%, about 40%,about 45%, about 50%, about 55%, about 60%, about 65%, about 70%, orabout 75%.

In some embodiments, the binder is present in the slurry at aconcentration of about 0.2% to about 10%. In some embodiments, thebinder is present in the slurry at a concentration of at least about0.2%. In some embodiments, the binder is present in the slurry at aconcentration of at most about 10%. In some embodiments, the binder ispresent in the slurry at a concentration of about 0.2% to about 0.5%,about 0.2% to about 0.75%, about 0.2% to about 1%, about 0.2% to about2%, about 0.2% to about 3%, about 0.2% to about 4%, about 0.2% to about5%, about 0.2% to about 6%, about 0.2% to about 7%, about 0.2% to about8%, about 0.2% to about 10%, about 0.5% to about 0.75%, about 0.5% toabout 1%, about 0.5% to about 2%, about 0.5% to about 3%, about 0.5% toabout 4%, about 0.5% to about 5%, about 0.5% to about 6%, about 0.5% toabout 7%, about 0.5% to about 8%, about 0.5% to about 10%, about 0.75%to about 1%, about 0.75% to about 2%, about 0.75% to about 3%, about0.75% to about 4%, about 0.75% to about 5%, about 0.75% to about 6%,about 0.75% to about 7%, about 0.75% to about 8%, about 0.75% to about10%, about 1% to about 2%, about 1% to about 3%, about 1% to about 4%,about 1% to about 5%, about 1% to about 6%, about 1% to about 7%, about1% to about 8%, about 1% to about 10%, about 2% to about 3%, about 2% toabout 4%, about 2% to about 5%, about 2% to about 6%, about 2% to about7%, about 2% to about 8%, about 2% to about 10%, about 3% to about 4%,about 3% to about 5%, about 3% to about 6%, about 3% to about 7%, about3% to about 8%, about 3% to about 10%, about 4% to about 5%, about 4% toabout 6%, about 4% to about 7%, about 4% to about 8%, about 4% to about10%, about 5% to about 6%, about 5% to about 7%, about 5% to about 8%,about 5% to about 10%, about 6% to about 7%, about 6% to about 8%, about6% to about 10%, about 7% to about 8%, about 7% to about 10%, or about8% to about 10%. In some embodiments, the binder is present in theslurry at a concentration of about 0.2%, about 0.5%, about 0.75%, about1%, about 2%, about 3%, about 4%, about 5%, about 6%, about 7%, about8%, or about 10%.

In some embodiments, the solvent is present in the slurry at aconcentration of about 5% to about 80%. In some embodiments, the solventis present in the slurry at a concentration of at least about 5%. Insome embodiments, the solvent is present in the slurry at aconcentration of at most about 80%. In some embodiments, the solvent ispresent in the slurry at a concentration of about 5% to about 10%, about5% to about 15%, about 5% to about 20%, about 5% to about 25%, about 5%to about 30%, about 5% to about 35%, about 5% to about 40%, about 5% toabout 50%, about 5% to about 60%, about 5% to about 70%, about 5% toabout 80%, about 10% to about 15%, about 10% to about 20%, about 10% toabout 25%, about 10% to about 30%, about 10% to about 35%, about 10% toabout 40%, about 10% to about 50%, about 10% to about 60%, about 10% toabout 70%, about 10% to about 80%, about 15% to about 20%, about 15% toabout 25%, about 15% to about 30%, about 15% to about 35%, about 15% toabout 40%, about 15% to about 50%, about 15% to about 60%, about 15% toabout 70%, about 15% to about 80%, about 20% to about 25%, about 20% toabout 30%, about 20% to about 35%, about 20% to about 40%, about 20% toabout 50%, about 20% to about 60%, about 20% to about 70%, about 20% toabout 80%, about 25% to about 30%, about 25% to about 35%, about 25% toabout 40%, about 25% to about 50%, about 25% to about 60%, about 25% toabout 70%, about 25% to about 80%, about 30% to about 35%, about 30% toabout 40%, about 30% to about 50%, about 30% to about 60%, about 30% toabout 70%, about 30% to about 80%, about 35% to about 40%, about 35% toabout 50%, about 35% to about 60%, about 35% to about 70%, about 35% toabout 80%, about 40% to about 50%, about 40% to about 60%, about 40% toabout 70%, about 40% to about 80%, about 50% to about 60%, about 50% toabout 70%, about 50% to about 80%, about 60% to about 70%, about 60% toabout 80%, or about 70% to about 80%. In some embodiments, the solventis present in the slurry at a concentration of about 5%, about 10%,about 15%, about 20%, about 25%, about 30%, about 35%, about 40%, about50%, about 60%, about 70%, or about 80%.

The process(ing) may start with un-winding an aluminum foil for coatinga slurry (e.g., of a formula) as shown in FIG. 4. FIG. 5 shows anexample of a close-up view of a slurry as it is being coated onto analuminum foil (slurry is black in color). The coated slurry may form afilm. The process(ing) may include drying of the coated film. FIG. 6shows an example of a coated film (e.g., a film comprising acarbon-based material, for example, PCS) of an electrode after drying at120° C. using an in-line heating oven. The process(ing) may includerewinding the aluminum foil after it has been coated. FIG. 7 shows anexample of rewinding an aluminum foil after it has been coated with thecarbon-based material (e.g., PCS).

A manufacturing process of a battery (e.g., an LFP-based cell) may be asillustrated in FIG. 10. A positive electrode (cathode during discharge)may be prepared from cathode material 1001 comprising PCS/LFP. Mixing1002 of the cathode material 1001 may be followed by coating and drying1004 on an aluminum foil 1003. The coated foil may be processed byslitting 1005 and in a roll press 1006. A negative electrode (anodeduring discharge) may be prepared from anode material 1011 comprisinggraphite. Mixing 1012 of the anode material 1011 may be followed bycoating and drying 1014 on a copper foil 1013. The coated foil may beprocessed by slitting 1015 and in a roll press 1016.

A separator 1021 may then be integrated with (e.g., disposed between)the positive and negative electrodes. Next, the process may includewinding 1022 of the positive electrode, negative electrode, andseparator. The wound roll may be placed in a can 1024, followed bywinding and necking 1023. Next, vacuum drying 1032 may be performed,followed by filling 1033 with an electrolyte 1034. A top can 1035 may beused for sealing 1036. The steps 1032, 1033, and 1036 may be performedin a dry room 1031. In some embodiments, the electrolyte 1034 and thetop cap 1035 may be prepared or stored in the dry room environment.Finally, the battery may be sent to labeling and testing 1041.

A manufacturing process of a battery (e.g., an NCA-based cell) may be asillustrated in FIG. 14. A positive electrode (cathode during discharge)may be prepared from cathode material 1401 comprising PCS/NCA. Mixing1402 of the positive electrode material may be followed by coating anddrying 1404 on an aluminum foil 1403. The coated foil may be processedby slitting 1405 and in a roll press 1406. A negative electrode (anodeduring discharge) may be prepared from anode material 1411 comprisinggraphite. Mixing 1412 of the anode material 1411 may be followed bycoating and drying 1414 on a copper foil 1413. The coated foil may beprocessed by slitting 1415 and in a roll press 1416.

A separator 1421 may then be integrated with (e.g., disposed between)the positive and negative electrodes. Next, the process may includewinding 1422 of the positive electrode, negative electrode, andseparator. The wound roll may be placed in a can 1424, followed bywinding and necking 1423. Next, vacuum drying 1432 may be performed,followed by filling 1433 with an electrolyte 1434. A top can 1435 may beused for sealing 1436. The steps 1432, 1433, and 1436 may be performedin a dry room 1431. In some embodiments, the electrolyte 1434 and thetop cap 1435 may be prepared or stored in the dry room environment.Finally, the battery may be sent to labeling and testing 1441.

In some embodiments, an assembly process of a battery (e.g., anNMC-based cell) may be as illustrated in FIGS. 18-20. The process mayinclude stacking (FIGS. 18-19), and/or winding or rolling (FIG. 20). Forexample, the battery may be assembled through stacking or winding.

FIG. 18 is a bird's eye view of stacking of a cell (e.g., an NMC-basedcell). Assembly may be performed on a jig 1807. The assembly may beperformed on a substrate 1800 (e.g., a wooden substrate). A metal rod1801 may confine the assembly of a positive electrode 1802 with analuminum foil current collector 1803, a separator 1804, and negativeelectrode 1805 with a copper foil current collector 1806. The positiveelectrode 1802 and aluminum foil current collector 1803 may be formed(at least in part) as described elsewhere herein (e.g., in relation toFIGS. 2-7, FIG. 10 and FIG. 14). The negative electrode 1805 and copperfoil current collector 1806 may be formed (at least in part) asdescribed elsewhere herein (e.g., in relation to FIGS. 2-7, FIG. 10 andFIG. 14).

FIG. 19 is a cross-sectional view of the stacking of a cell (e.g., anNMC-based cell). Assembly may be performed on a jig 1907. Assembly maybe performed on a substrate 1900 (e.g., a wooden substrate). A separator1901 may be laid first, thereby creating a first layer of the separator.The separator may be unwound as shown in FIG. 19 and held in place bythe jig. A positive electrode (e.g., positive electrode comprising orcoupled to an aluminum foil serving as a positive current collector)1902 may be placed on top of the first layer of the separator 1901(left). Next, the separator may be folded over the positive electrode1902 to create a second layer of the separator, and a negative electrode(e.g., negative electrode comprising or coupled to a copper foil servingas a negative current collector) 1912 may be placed on top of the secondlayer of the separator 1911 (right). The negative and positiveelectrodes (e.g., including current collectors) may be formed (at leastin part) as described elsewhere herein (e.g., in relation to FIGS. 2-7,FIG. 10, and FIG. 14).

FIG. 20 is an example of the winding of a cell (e.g., an NMC-basedcell). Layered sheets including a first sheet of a separator 2001, apositive electrode 2002, a second sheet of the separator 2003, and anegative electrode 2004 may be rotated along an axis 2000 to form thecell. The negative and positive electrodes (e.g., including currentcollectors) may be formed (at least in part) as described elsewhereherein (e.g., in relation to FIGS. 2-7, FIG. 10 and FIG. 14).

One or more steps of the fabrication process in FIG. 2 and/or one ormore of the processing steps in FIGS. 3-7 may be used to producefinished products (batteries) such as shown in FIG. 11, FIG. 15, andFIG. 21.

Performance of Energy Storage Devices

Energy storage devices available in the market may provide around 1000mAh of charge storage capacity, power density of 500-1500 watts perkilogram (W/kg), and cycling stability of 500 cycles. However, furtherimprovements of these figures are necessary for the wide adoption ofthis technology, especially for large scale applications such aselectric vehicles and grid scale energy storage (e.g., to reduce theprice of electric vehicles and contribute to a clean and greenenvironment).

In contrast, the energy storage devices (e.g., batteries) providedherein may in some embodiments provide a capacity (e.g., charge storagecapacity) of more than 2200 or 3400 mAh and a power density of around3000 W/kg and be used for more than 1000 cycles. Such features may beenabled, for example, by outstanding electrical and mechanicalproperties of the carbon-based materials described herein,extraordinarily high surface area of the carbon-based materialsdescribed herein, or a combination thereof. The carbon-based materialsdescribed herein may make the energy storage devices (e.g., batteries)lighter, more powerful, more efficient, or any combination thereof.

FIG. 12 shows example performance of an LFP-based battery. FIG. 22 showsexample performance of an NMC-based battery.

Per FIG. 26, an energy storage device (e.g., battery or battery cell) ofthe present disclosure may have a charge storage capacity of at leastabout 1.5, 2, 2.1, 2.2, 2.3, 2.4, 2.5, 2.6, 2.7, 2.8, 2.9, or 3 timesgreater than an LIB available in the market (e.g., an LIB with a chargestorage capacity of 1000 or 3400 mAh). Exemplary LIBs currentlyavailable in the market, per FIG. 26, comprise the NCR-18650A, theNCR-18650B, and the NCR-18650PF LIBs made by Panasonic, as well as theINR-18650-25R LIB made by Samsung. An energy storage device (e.g.,battery or battery cell) of the present disclosure may have a powerdensity at least about 1.5, 2, 2.5, 3, 3.5, 4, 4.5, 5, 5.5, 6, 6.5, 7,7.5, or 8 times greater than an LIB available in the market (e.g., anLIB with a power density of 500-1500 W/kg). An energy storage device(e.g., battery or battery cell) of the present disclosure may havecycling stability or cycle life at least about 1.5, 2, or 2.5 timesgreater than an LIB available in the market (e.g., an LIB with a cyclingstability or cycle life of 500 or 1000 cycles). For example, an energystorage device (e.g., battery or battery cell) of the present disclosuremay run electronic device(s) for twice as long and may be used for morethan 1000 cycles compared with only 500 cycles for competitivetechnologies. In some embodiments, a battery of the present disclosurenot only may have a much higher capacity than commercial cells but alsomay provide high power and last longer. An energy storage device (e.g.,battery or battery cell) of the present disclosure may have an energydensity at least about 1.5, 2, or 2.5 times greater than an LIBavailable in the market (e.g., an LIB with an energy density of 90-150watt-hour per kilogram (Wh/kg)). An energy storage device (e.g., batteryor battery cell) of the present disclosure may be at least about 2 timesmore powerful (e.g., at least 2 times greater charge storage capacity,at least 2 times greater power density, and/or at least 2 times greatercycling stability/cycle life) than commercial (e.g., LIB) cells.

An energy storage device (e.g., battery or battery cell) of the presentdisclosure may have a charge storage capacity of greater than or equalto about 750 mAh, 800 mAh, 850 mAh, 950 mAh, 1000 mAh, 1100 mAh, 1200mAh, 1300 mAh, 1400 mAh, 1500 mAh, 1600 mAh, 1700 mAh, 1800 mAh, 1900mAh, 2000 mAh, 2100 mAh, 2200 mAh, 2300 mAh, 2400 mAh, 2500 mAh, 2600mAh, 2700 mAh, 2800 mAh, 2900 mAh, 3000 mAh, 3100 mAh, 3200 mAh, 3300mAh, 3400 mAh, 3500 mAh, 3600 mAh, 3700 mAh, 3800 mAh, 3900 mAh, 4000mAh, 4200 mAh, 4600 mAh, 4800 mAh, 5000 mAh. An energy storage device(e.g., battery or battery cell) of the present disclosure may have acharge storage capacity between about 1000 mAh and 2500 mAh, 1000 mAhand 3000 mAh, 1000 mAh and 3500 mAh, 1000 mAh and 4000 mAh, 1100 mAh and2500 mAh, 1100 mAh and 3000 mAh, 1100 mAh and 3500 mAh, 1100 mAh and4000 mAh, 1200 mAh and 2500 mAh, 1200 mAh and 3000 mAh, 1200 mAh and3500 mAh, 1200 mAh and 4000 mAh, 1300 mAh and 2500 mAh, 1300 mAh and3000 mAh, 1300 mAh and 3500 mAh, 1300 mAh and 4000 mAh, 1400 mAh and2500 mAh, 1400 mAh and 3000 mAh, 1400 mAh and 3500 mAh, 1400 mAh and4000 mAh, 1500 mAh and 2500 mAh, 1500 mAh and 3000 mAh, 1500 mAh and3500 mAh, 1500 mAh and 4000 mAh, 1600 mAh and 2500 mAh, 1600 mAh and3000 mAh, 1600 mAh and 3500 mAh, 1600 mAh and 4000 mAh, 1700 mAh and2500 mAh, 1700 mAh and 3000 mAh, 1700 mAh and 3500 mAh, 1700 mAh and4000 mAh, 1800 mAh and 2500 mAh, 1800 mAh and 3000 mAh, 1800 mAh and3500 mAh, 1800 mAh and 4000 mAh, 1900 mAh and 2500 mAh, 1900 mAh and3000 mAh, 1900 mAh and 3500 mAh, 1900 mAh and 4000 mAh, 2000 mAh and2500 mAh, 2000 mAh and 3000 mAh, 2000 mAh and 3500 mAh, 2000 mAh and4000 mAh, 2500 mAh and 3000 mAh, 2500 mAh and 3500 mAh, 2500 mAh and4000 mAh, 3000 mAh and 3500 mAh, 3000 mAh and 4000 mAh, or 3500 mAh and4000 mAh. An energy storage device (e.g., battery or battery cell) ofthe present disclosure may have such charge storage capacities incombination with one or more power densities, energy densities, and/orcycling stabilities/cycle lives described herein. In some embodiments,an energy storage device (e.g., battery or battery cell) of the presentdisclosure has a storage capacity of about 800 mAh to about 4,000 mAh.In some embodiments, an energy storage device (e.g., battery or batterycell) of the present disclosure has a storage capacity of at least about1,000 mAh.

An energy storage device (e.g., battery or battery cell) of the presentdisclosure may have a charge storage capacity of about 80 mAh/g to about800 mAh/g. An energy storage device (e.g., battery or battery cell) ofthe present disclosure may have a charge storage capacity of at leastabout 80 mAh/g. An energy storage device (e.g., battery or battery cell)of the present disclosure may have a charge storage capacity of at mostabout 800 mAh/g. An energy storage device (e.g., battery or batterycell) of the present disclosure may have a charge storage capacity ofabout 80 mAh/g to about 100 mAh/g, about 80 mAh/g to about 150 mAh/g,about 80 mAh/g to about 200 mAh/g, about 80 mAh/g to about 300 mAh/g,about 80 mAh/g to about 400 mAh/g, about 80 mAh/g to about 500 mAh/g,about 80 mAh/g to about 600 mAh/g, about 80 mAh/g to about 700 mAh/g,about 80 mAh/g to about 800 mAh/g, about 100 mAh/g to about 150 mAh/g,about 100 mAh/g to about 200 mAh/g, about 100 mAh/g to about 300 mAh/g,about 100 mAh/g to about 400 mAh/g, about 100 mAh/g to about 500 mAh/g,about 100 mAh/g to about 600 mAh/g, about 100 mAh/g to about 700 mAh/g,about 100 mAh/g to about 800 mAh/g, about 150 mAh/g to about 200 mAh/g,about 150 mAh/g to about 300 mAh/g, about 150 mAh/g to about 400 mAh/g,about 150 mAh/g to about 500 mAh/g, about 150 mAh/g to about 600 mAh/g,about 150 mAh/g to about 700 mAh/g, about 150 mAh/g to about 800 mAh/g,about 200 mAh/g to about 300 mAh/g, about 200 mAh/g to about 400 mAh/g,about 200 mAh/g to about 500 mAh/g, about 200 mAh/g to about 600 mAh/g,about 200 mAh/g to about 700 mAh/g, about 200 mAh/g to about 800 mAh/g,about 300 mAh/g to about 400 mAh/g, about 300 mAh/g to about 500 mAh/g,about 300 mAh/g to about 600 mAh/g, about 300 mAh/g to about 700 mAh/g,about 300 mAh/g to about 800 mAh/g, about 400 mAh/g to about 500 mAh/g,about 400 mAh/g to about 600 mAh/g, about 400 mAh/g to about 700 mAh/g,about 400 mAh/g to about 800 mAh/g, about 500 mAh/g to about 600 mAh/g,about 500 mAh/g to about 700 mAh/g, about 500 mAh/g to about 800 mAh/g,about 600 mAh/g to about 700 mAh/g, about 600 mAh/g to about 800 mAh/g,or about 700 mAh/g to about 800 mAh/g. An energy storage device (e.g.,battery or battery cell) of the present disclosure may have a chargestorage capacity of about 80 mAh/g, about 100 mAh/g, about 150 mAh/g,about 200 mAh/g, about 300 mAh/g, about 400 mAh/g, about 500 mAh/g,about 600 mAh/g, about 700 mAh/g, about 800 mAh/g, or about 80 mAh/g.

An energy storage device (e.g., battery or battery cell) of the presentdisclosure may have such charge storage capacities in combination withone or more power densities, energy densities, and/or cyclingstabilities/cycle lives described herein. In some embodiments, an energystorage device (e.g., battery or battery cell) of the present disclosurehas a storage capacity of about 80 mAh/g to about 800 mAh/g. In someembodiments, an energy storage device (e.g., battery or battery cell) ofthe present disclosure has a storage capacity of at least about 1,000mAh/g.

An energy storage device (e.g., battery or battery cell) of the presentdisclosure may have a power density of greater than or equal to about500 W/kg, 600 W/kg, 700 W/kg, 800 W/kg, 900 W/kg, 1000 W/kg, 1100 W/kg,1200 W/kg, 1300 W/kg, 1400 W/kg, 1500 W/kg, 1600 W/kg, 1700 W/kg, 1800W/kg, 1900 W/kg, 2000 W/kg, 2100 W/kg, 2200 W/kg, 2300 W/kg, 2400 W/kg,2500 W/kg, 2600 W/kg, 2700 W/kg, 2800 W/kg, 2900 W/kg, 3000 W/kg, 3100W/kg, 3200 W/kg, 3300 W/kg, 3400 W/kg, or 3500 W/kg. An energy storagedevice (e.g., battery or battery cell) of the present disclosure mayhave a power density between about 500 W/kg and 3000 W/kg, 500 W/kg and3500 W/kg, 1000 W/kg and 3000 W/kg, 1000 W/kg and 3500 W/kg, 1500 W/kgand 3000 W/kg, 1500 W/kg and 3500 W/kg, 1600 W/kg and 3000 W/kg, 1600W/kg and 3500 W/kg, 1700 W/kg and 3000 W/kg, 1700 W/kg and 3500 W/kg,1800 W/kg and 3000 W/kg, 1800 W/kg and 3500 W/kg, 1900 W/kg and 3000W/kg, 1900 W/kg and 3500 W/kg, 2000 W/kg and 3000 W/kg, 2000 W/kg and3500 W/kg, 2100 W/kg and 3000 W/kg, 2100 W/kg and 3500 W/kg, 2200 W/kgand 3000 W/kg, 2200 W/kg and 3500 W/kg, 2300 W/kg and 3000 W/kg, 2300W/kg and 3500 W/kg, 2400 W/kg and 3000 W/kg, 2400 W/kg and 3500 W/kg,2500 W/kg and 3000 W/kg, 2500 W/kg and 3500 W/kg, 2600 W/kg and 3000W/kg, 2600 W/kg and 3500 W/kg, 2700 W/kg and 3000 W/kg, 2700 W/kg and3500 W/kg, 2800 W/kg and 3000 W/kg, 2800 W/kg and 3500 W/kg, 2900 W/kgand 3000 W/kg, 2900 W/kg and 3500 W/kg, or 3000 W/kg and 3500 W/kg. Anenergy storage device (e.g., battery or battery cell) of the presentdisclosure may have such power densities in combination with one or morecharge storage capacities, energy densities, and/or cyclingstabilities/cycle lives described herein.

An energy storage device (e.g., battery or battery cell) of the presentdisclosure may have a cycling stability or cycle life of greater than orequal to about 500 cycles, 600 cycles, 700 cycles, 800 cycles, 900cycles, 1000 cycles, 1100 cycles, 1200 cycles, 1300 cycles, 1400 cycles,1500 cycles, or 2000 cycles. An energy storage device (e.g., battery orbattery cell) of the present disclosure may have a cycling stability orcycle life between about 500 cycles and 1000 cycles, 500 cycles and 1500cycles, 600 cycles and 1000 cycles, 600 cycles and 1500 cycles, 700cycles and 1000 cycles, 700 cycles and 1500 cycles, 800 cycles and 1000cycles, 800 cycles and 1500 cycles, 800 cycles and 1000 cycles, 800cycles and 1500 cycles, 900 cycles and 1000 cycles, 900 cycles and 1500cycles, 1000 cycles and 1500 cycles, or 1500 cycles and 2000 cycles. Anenergy storage device (e.g., battery or battery cell) of the presentdisclosure may have such cycling stabilities/cycle lives in combinationwith one or more charge storage capacities, power densities and/orenergy densities described herein.

An energy storage device (e.g., battery or battery cell) of the presentdisclosure may have an energy density of greater than or equal to about50 Wh/kg, 75 Wh/kg, 90 Wh/kg, 100 Wh/kg, 110 Wh/kg, 120 Wh/kg, 130Wh/kg, 140 Wh/kg, 150 Wh/kg, 160 Wh/kg, 170 Wh/kg, 180 Wh/kg, 190 Wh/kg,200 Wh/kg, 210 Wh/kg, 220 Wh/kg, 230 Wh/kg, 240 Wh/kg, 250 Wh/kg, 260Wh/kg, 270 Wh/kg, 280 Wh/kg, 290 Wh/kg, 300 Wh/kg, 310 Wh/kg, 320 Wh/kg,330 Wh/kg, 340 Wh/kg, 350 Wh/kg, 360 Wh/kg, 370 Wh/kg, 380 Wh/kg, 390Wh/kg or 400 Wh/kg. An energy storage device (e.g., battery or batterycell) of the present disclosure may have an energy density between about90 Wh/kg and 250 Wh/kg, 90 Wh/kg and 300 Wh/kg, 90 Wh/kg and 350 Wh/kg,90 Wh/kg and 400 Wh/kg, 150 Wh/kg and 250 Wh/kg, 150 Wh/kg and 300Wh/kg, 150 Wh/kg and 350 Wh/kg, 150 Wh/kg and 400 Wh/kg, 200 Wh/kg and250 Wh/kg, 200 Wh/kg and 300 Wh/kg, 200 Wh/kg and 350 Wh/kg, 200 Wh/kgand 400 Wh/kg, 250 Wh/kg and 300 Wh/kg, 250 Wh/kg and 350 Wh/kg, 250Wh/kg and 400 Wh/kg, 300 Wh/kg and 350 Wh/kg, 300 Wh/kg and 400 Wh/kg,or 350 Wh/kg and 400 Wh/kg. An energy storage device (e.g., battery orbattery cell) of the present disclosure may have such energy densitiesin combination with one or more charge storage capacities, powerdensities, and/or cycling stabilities/cycle lives described herein.

An energy storage device (e.g., battery or battery cell) of the presentdisclosure may have a charge voltage of greater than or equal to about 2V, 2.1 V, 2.2 V, 2.3 V, 2.4 V, 2.5 V, 2.6 V, 2.7 V, 2.8 V, 2.9 V, 3 V,3.1 V, 3.2 V, 3.3 V, 3.4 V, 3.5 V, 3.6 V, 3.7 V, 3.8 V, 3.9 V, 4 V, 4.1V, 4.2 V, 4.3 V, 4.4 V, or 4.5 V. An energy storage device (e.g.,battery or battery cell) of the present disclosure may have a chargevoltage between about 2 V and 2.5 V, 2 V and 3 V, 2 V and 3.5 V, 2 V and4 V, 2 V and 4.5 V, 2.5 V and 3 V, 2.5 V and 3.5 V, 2.5 V and 4 V, 2.5 Vand 4.5 V, 3 V and 3.5 V, 3 V and 4 V, 3 V and 4.5 V, 3.5 V and 4 V, 3.5V and 4.5 V, or 4 V and 4.5 V. An energy storage device (e.g., batteryor battery cell) of the present disclosure may have a discharge voltageof greater than or equal to about 2 V, 2.5 V, 3 V, 3.5 V, 4 V, or 4.5 V.An energy storage device (e.g., battery or battery cell) of the presentdisclosure may a discharge voltage between about 2 V and 2.5 V, 2 V and3 V, 2 V and 3.5 V, 2 V and 4 V, 2 V and 4.5 V, 2.5 V and 3 V, 2.5 V and3.5 V, 2.5 V and 4 V, 2.5 V and 4.5 V, 3 V and 3.5 V, 3 V and 4 V, 3 Vand 4.5 V, 3.5 V and 4 V, 3.5 V and 4.5 V, or 4 V and 4.5 V. In someembodiments, the charge and discharge voltage may differ by less than orequal to about 25%, 20%, 15%, 10% or 5% (e.g., see FIG. 12). The chargeand discharge voltage may have such similarities over a given capacityrange (e.g., up to about 1000 mAh, 1100 mAh, 1200 mAh, 1300 mAh, 1400mAh, 1600 mAh, 1700 mAh, 1800 mAh, 1900 mAh, 2000 mAh, 2200 mAh, 2400mAh, 2600 mAh, 2800 mAh, 3000 mAh, 3200 mAh, 3400 mAh, 3600 mAh, 3800mAh or 4000 mAh).

Per FIG. 27, energy storage devices available in the market exhibit anequivalent series resistance (ESR) of about 40Ω to about 70Ω. However,further improvements of these figures are necessary for the wideadoption of this technology, especially for large scale applicationssuch as electric vehicles and grid scale energy storage (e.g., to reducethe price of electric vehicles and contribute to a clean and greenenvironment).

In contrast, the energy storage devices (e.g., batteries) providedherein may in some embodiments exhibit an ESR of less than 30Ω, ascalculated by the potential-time graph in FIG. 28. Such features may beenabled, for example, by outstanding electrical and mechanicalproperties of the carbon-based materials described herein,extraordinarily high surface area of the carbon-based materialsdescribed herein, or a combination thereof.

An energy storage device (e.g., battery or battery cell) of the presentdisclosure may have an ESR at 1 kilohertz (kHz) of 14 milliohms to 80milliohms. An energy storage device (e.g., battery or battery cell) ofthe present disclosure may have an ESR at 1 kHz of at least 14milliohms. An energy storage device (e.g., battery or battery cell) ofthe present disclosure may have an ESR at 1 kHz of at most 80 milliohms.An energy storage device (e.g., battery or battery cell) of the presentdisclosure may have an ESR at 1 kHz of 14 milliohms to 20 milliohms, 14milliohms to 25 milliohms, 14 milliohms to 30 milliohms, 14 milliohms to35 milliohms, 14 milliohms to 40 milliohms, 14 milliohms to 45milliohms, 14 milliohms to 50 milliohms, 14 milliohms to 55 milliohms,14 milliohms to 60 milliohms, 14 milliohms to 70 milliohms, 14 milliohmsto 80 milliohms, 20 milliohms to 25 milliohms, 20 milliohms to 30milliohms, 20 milliohms to 35 milliohms, 20 milliohms to 40 milliohms,20 milliohms to 45 milliohms, 20 milliohms to 50 milliohms, 20 milliohmsto 55 milliohms, 20 milliohms to 60 milliohms, 20 milliohms to 70milliohms, 20 milliohms to 80 milliohms, 25 milliohms to 30 milliohms,25 milliohms to 35 milliohms, 25 milliohms to 40 milliohms, 25 milliohmsto 45 milliohms, 25 milliohms to 50 milliohms, 25 milliohms to 55milliohms, 25 milliohms to 60 milliohms, 25 milliohms to 70 milliohms,25 milliohms to 80 milliohms, 30 milliohms to 35 milliohms, 30 milliohmsto 40 milliohms, 30 milliohms to 45 milliohms, 30 milliohms to 50milliohms, 30 milliohms to 55 milliohms, 30 milliohms to 60 milliohms,30 milliohms to 70 milliohms, 30 milliohms to 80 milliohms, 35 milliohmsto 40 milliohms, 35 milliohms to 45 milliohms, 35 milliohms to 50milliohms, 35 milliohms to 55 milliohms, 35 milliohms to 60 milliohms,35 milliohms to 70 milliohms, 35 milliohms to 80 milliohms, 40 milliohmsto 45 milliohms, 40 milliohms to 50 milliohms, 40 milliohms to 55milliohms, 40 milliohms to 60 milliohms, 40 milliohms to 70 milliohms,40 milliohms to 80 milliohms, 45 milliohms to 50 milliohms, 45 milliohmsto 55 milliohms, 45 milliohms to 60 milliohms, 45 milliohms to 70milliohms, 45 milliohms to 80 milliohms, 50 milliohms to 55 milliohms,50 milliohms to 60 milliohms, 50 milliohms to 70 milliohms, 50 milliohmsto 80 milliohms, 55 milliohms to 60 milliohms, 55 milliohms to 70milliohms, 55 milliohms to 80 milliohms, 60 milliohms to 70 milliohms,60 milliohms to 80 milliohms, or 70 milliohms to 80 milliohms. An energystorage device (e.g., battery or battery cell) of the present disclosuremay have an ESR at 1 kHz of 14 milliohms, 20 milliohms, 25 milliohms, 30milliohms, 35 milliohms, 40 milliohms, 45 milliohms, 50 milliohms, 55milliohms, 60 milliohms, 70 milliohms, or 80 milliohms. An energystorage device (e.g., battery or battery cell) of the present disclosuremay have an ESR at 1 kHz of about 5 milliohms to about 100 milliohms. Anenergy storage device (e.g., battery or battery cell) of the presentdisclosure may have an ESR at 1 kHz of at least about 5 milliohms. Anenergy storage device (e.g., battery or battery cell) of the presentdisclosure may have an ESR at 1 kHz of at most about 100 milliohms. Anenergy storage device (e.g., battery or battery cell) of the presentdisclosure may have an ESR at 1 kHz of about 5 milliohms to about 10milliohms, about 5 milliohms to about 20 milliohms, about 5 milliohms toabout 30 milliohms, about 5 milliohms to about 40 milliohms, about 5milliohms to about 50 milliohms, about 5 milliohms to about 60milliohms, about 5 milliohms to about 70 milliohms, about 5 milliohms toabout 80 milliohms, about 5 milliohms to about 90 milliohms, about 5milliohms to about 100 milliohms, about 10 milliohms to about 20milliohms, about 10 milliohms to about 30 milliohms, about 10 milliohmsto about 40 milliohms, about 10 milliohms to about 50 milliohms, about10 milliohms to about 60 milliohms, about 10 milliohms to about 70milliohms, about 10 milliohms to about 80 milliohms, about 10 milliohmsto about 90 milliohms, about 10 milliohms to about 100 milliohms, about20 milliohms to about 30 milliohms, about 20 milliohms to about 40milliohms, about 20 milliohms to about 50 milliohms, about 20 milliohmsto about 60 milliohms, about 20 milliohms to about 70 milliohms, about20 milliohms to about 80 milliohms, about 20 milliohms to about 90milliohms, about 20 milliohms to about 100 milliohms, about 30 milliohmsto about 40 milliohms, about 30 milliohms to about 50 milliohms, about30 milliohms to about 60 milliohms, about 30 milliohms to about 70milliohms, about 30 milliohms to about 80 milliohms, about 30 milliohmsto about 90 milliohms, about 30 milliohms to about 100 milliohms, about40 milliohms to about 50 milliohms, about 40 milliohms to about 60milliohms, about 40 milliohms to about 70 milliohms, about 40 milliohmsto about 80 milliohms, about 40 milliohms to about 90 milliohms, about40 milliohms to about 100 milliohms, about 50 milliohms to about 60milliohms, about 50 milliohms to about 70 milliohms, about 50 milliohmsto about 80 milliohms, about 50 milliohms to about 90 milliohms, about50 milliohms to about 100 milliohms, about 60 milliohms to about 70milliohms, about 60 milliohms to about 80 milliohms, about 60 milliohmsto about 90 milliohms, about 60 milliohms to about 100 milliohms, about70 milliohms to about 80 milliohms, about 70 milliohms to about 90milliohms, about 70 milliohms to about 100 milliohms, about 80 milliohmsto about 90 milliohms, about 80 milliohms to about 100 milliohms, orabout 90 milliohms to about 100 milliohms. An energy storage device(e.g., battery or battery cell) of the present disclosure may have anESR at 1 kHz of about 5 milliohms, about 10 milliohms, about 20milliohms, about 30 milliohms, about 40 milliohms, about 50 milliohms,about 60 milliohms, about 70 milliohms, about 80 milliohms, about 90milliohms, or about 100 milliohms.

Terms and Definitions

Unless otherwise defined, all technical terms used herein have the samemeaning as commonly understood by one of ordinary skill in the art towhich the present disclosure belongs. As used in this specification andthe appended claims, the singular forms “a,” “an,” and “the” includeplural references unless the context clearly dictates otherwise. Anyreference to “or” herein is intended to encompass “and/or” unlessotherwise stated.

While preferable embodiments of the present disclosure have been shownand described herein, it will be obvious to those skilled in the artthat such embodiments are provided by way of example only. Numerousvariations, changes, and substitutions will now occur to those skilledin the art without departing from the present disclosure. It should beunderstood that various alternatives to the embodiments of the device ofthe present disclosure described herein may be employed in practicingthe present disclosure. It is intended that the following claims definethe scope of the present disclosure and that methods and structureswithin the scope of these claims and their equivalents be coveredthereby.

Throughout the present disclosure, numerical features are presented in arange format. It should be understood that the description in rangeformat is merely for convenience and brevity and should not be construedas an inflexible limitation on the scope of any embodiments.Accordingly, the description of a range should be considered to havespecifically disclosed all the possible subranges as well as individualnumerical values within that range to the tenth of the unit of the lowerlimit unless the context clearly dictates otherwise. For example,description of a range such as from 1 to 6 should be considered to havespecifically disclosed subranges such as from 1 to 3, from 1 to 4, from1 to 5, from 2 to 4, from 2 to 6, and from 3 to 6, as well as individualvalues within that range, for example, 1.1, 2, 2.3, 5, and 5.9. Thisapplies regardless of the breadth of the range. The upper and lowerlimits of these intervening ranges may independently be included in thesmaller ranges, and are also encompassed within the present disclosure,subject to any specifically excluded limit in the stated range. Wherethe stated range includes one or both of the limits, ranges excludingeither or both of those included limits are also included in the presentdisclosure, unless the context clearly dictates otherwise.

Unless specifically stated or obvious from context, as used herein, theterm “about” in reference to a number or range of numbers is understoodto mean the stated number and numbers ±10% thereof, or 10% below thelower listed limit and 10% above the higher listed limit for the valueslisted for a range.

EXAMPLES Example 1—NCA Cell

An exemplary battery comprises at least one cell comprising a negativeelectrode (anode during discharge) comprising graphite and a positiveelectrode (cathode during discharge) comprising PCS/lithium nickelcobalt aluminum oxide (NCA), as shown in Table 1.

TABLE 1 NCA Cell Dry Wet Slurry Electrode Electrode Component MaterialComposition Composition Positive Active Graphene 0.3%-0.6% 0.5%-1%  Electrode electrode Lithium nickel 58%-59% 96%-97% material cobaltaluminum oxide Binder Polyvinylidene 1.5%  2.5%   fluoride SolventN-methyl-2- 39% 0% pyrrolidone Negative Active Natural graphite 49% 95% Electrode material Conductive Carbon Black 0.5%  1% additive Super-PBinder Polyvinylidene  2% 5% fluoride Solvent N-methyl-2- 48% 0%pyrrolidone

Example 2—NMC Cell

An exemplary battery comprises at least one cell comprising a negativeelectrode (anode during discharge) comprising graphite and a positiveelectrode (cathode during discharge) comprising PCS/lithium nickelmanganese cobalt oxide (NMC), as shown in Table 2.

TABLE 2 NMC Cell Dry Wet Slurry Electrode Electrode Component MaterialComposition Composition Positive Active Graphene 0.3%-0.6% 0.5%-1%  Electrode electrode Lithium nickel 58%-59% 96%-97% material manganesecobalt oxide Binder Polyvinylidene 1.5%  2.5%   fluoride SolventN-methyl-2- 39% 0% pyrrolidone Negative Active Natural graphite 49% 95% Electrode material Conductive Carbon Black 0.5%  1% additive Super-PBinder Polyvinylidene  2% 5% fluoride Solvent N-methyl-2- 48% 0%pyrrolidone

Example 3—LFP Cell

An exemplary battery comprises at least one cell comprising a negativeelectrode (anode during discharge) comprising graphite and a positiveelectrode (cathode during discharge) comprising PCS/lithium ironphosphate (LFP), as shown in Table 3.

TABLE 3 LFP Cell Dry Wet Slurry Electrode Electrode Component MaterialComposition Composition Positive Active Graphene 0.3%-0.6% 0.5%-1%  Electrode electrode Lithium iron 58%-59% 96%-97% material phosphateBinder Polyvinylidene 1.5%  2.5%   fluoride Solvent N-methyl-2- 39% 0%pyrrolidone Negative Active Natural graphite 49% 95%  Electrode materialConductive Carbon Black 0.5%  1% additive Super-P Binder Polyvinylidene 2% 5% fluoride Solvent N-methyl-2- 48% 0% pyrrolidone

What is claimed is:
 1. An energy storage device comprising: a) anegative electrode comprising: i) graphene; ii) a first binder; and iii)a conductive additive; b) a positive electrode comprising: i) an activematerial; and ii) a second binder; and c) a separator between thenegative electrode and the positive electrode.
 2. The device of claim 1,wherein at least one of the first binder and the second binder comprisespolyvinyl fluoride, polyvinylidene fluoride, polytetrafluoroethylene,polychlorotrifluoroethylene, perfluoroalkoxy polymer, fluorinatedethylene-propylene, polyethylenetetrafluoroethylene,polyethylenechlorotrifluoroethylene, perfluorinated plastomer, afluorocarbon, chlorotrifluoroethylenevinylidene fluoride, afluoroelastomer, tetrafluoroethylene-propylene, perfluoropolyether,perfluorosulfonic acid, perfluoropolyoxetane, P(VDF-trifluoroethylene),P(VDF-tetrafluoroethylene), or any combination thereof.
 3. The device ofclaim 1, wherein the conductive additive comprises carbon black,acetylene black, furnace black, vapor-grown carbon fibers, carbonnanotubes, porous carbon sheets, or any combination thereof.
 4. Thedevice of claim 1, wherein the active material comprises lithium ironphosphate, lithium nickel cobalt aluminum oxide, lithium nickelmanganese cobalt oxide, lithium cobalt oxide, lithium manganese oxide,lithium titanate, lithium sulfur, or any combination thereof.
 5. Thedevice of claim 1, having a storage capacity of about 800 milliamp hours(mAh) to about 4,000 mAh.
 6. The device of claim 1, having a storagecapacity of at least about 800 mAh.
 7. The device of claim 1, having astorage capacity of about 80 mAh/g to about 800 mAh/g.
 8. The device ofclaim 1, having a storage capacity of at least about 80 mAh/g.
 9. Thedevice of claim 1, having a cycle life of about 500 cycles to about 1500cycles.
 10. The device of claim 1, having a cycle life of at least about500 cycles.
 11. The device of claim 1, having an equivalent seriesresistance of about 5 milliohms to about 100 milliohms.
 12. The deviceof claim 1, having an equivalent series resistance of at most about 100milliohms.
 13. A method of fabricating an electrode comprising: a)combining a binder and a solvent; b) heating the binder and the solvent;c) mixing an active material into the binder and the solvent to form aslurry; d) roll coating the slurry onto a foil; e) drying the slurry onthe foil; f) roll pressing the slurry on the foil; g) slitting theslurry on the foil.
 14. The method of claim 13, wherein the bindercomprises polyvinyl fluoride, polyvinylidene fluoride,polytetrafluoroethylene, polychlorotrifluoroethylene, perfluoroalkoxypolymer, fluorinated ethylene-propylene,polyethylenetetrafluoroethylene, polyethylenechlorotrifluoroethylene,perfluorinated plastomer, a fluorocarbon,chlorotrifluoroethylenevinylidene fluoride, a fluoroelastomer,tetrafluoroethylene-propylene, perfluoropolyether, perfluorosulfonicacid, perfluoropolyoxetane, P(VDF-trifluoroethylene),P(VDF-tetrafluoroethylene), or any combination thereof.
 15. The methodof claim 13, wherein the solvent comprises 2-pyrrolidone,n-vinylpyrrolidone, n-methyl-2-pyrrolidone, methyl ethyl ketone, or anycombination thereof.
 16. The method of claim 13, wherein the activematerial comprises a lithiated metal compound and a carbon-basedmaterial.
 17. The method of claim 16, wherein the lithiated metalcompound comprises lithium nickel cobalt aluminum oxide, lithium nickelmanganese cobalt oxide, lithium iron phosphate, or any combinationthereof.
 18. The method of claim 16, wherein the carbon-based materialcomprises a porous carbon sheet, graphite, or any combination thereof.19. The method of claim 13, wherein the active material is present inthe slurry at a concentration of 40% to 60%.
 20. The method of claim 13,wherein the active material is present in the electrode at aconcentration of 50% to 90%.
 21. The method of claim 13, wherein thebinder is present in the slurry at a concentration of about 0.5% toabout 10%.
 22. The method of claim 13, wherein the binder is present inthe electrode at a concentration of about 1% to about 15%.
 23. Themethod of claim 13, wherein the solvent is present in the slurry at aconcentration of about 10% to 60%.